subject:(Water gas shift)

University of Bath

1. Williamson, David. Nanostructured catalysts for conversion of CO2 into hydrocarbons.

Degree: PhD, 2020, University of Bath

URL: https://researchportal.bath.ac.uk/en/studentthesis/nanostructured-catalysts-for-conversion-of-co2-into-hydrocarbons(60b3567d-d95a-417e-9029-ab06ba68a963).html ; https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.805662

► Increasing greenhouse gas emissions since the onset of industrialisation now pose a significant threat to modern society and the habitability our planet for future generations.… (more)

▼ Increasing greenhouse gas emissions since the onset of industrialisation now pose a significant threat to modern society and the habitability our planet for future generations. It has been determined that we must achieve zero net emissions by 2050 with a 45% decrease in emissions by 2030 (relative to 2010 levels) in order to limit warming to 1.5 °C by the end of the century. A wide variety of solutions are being explored to limit the impact of modern emissions and transition to a more sustainable energy infrastructure. One such example is the capture, storage and conversion of CO2 into valuable products and fuels for emissions mitigation and energy storage. Iron nanoparticles supported on carbon nanotubes known as [email protected] have proven themselves to be active for the catalytic hydrogenation of CO2 into hydrocarbons. This is due to their ability to catalyse both the reverse water-gas shift and Fischer-Tropsch processes, resulting in a coupled process that generates chemical fuels directly from a feed gas of hydrogen and CO2. Furthermore, the integration of the iron particles into the carbon nanotube support structure during synthesis results in a nanotube-particle bridged structure that enhances catalyst activity due to improved hydrogen spillover. However, the distribution of the resulting products is notoriously difficult to control, often requiring the addition of promoter metals to enhance catalyst activity and selectivity towards desirable products. These promoters are typically doped onto the surface of the catalyst using a wet impregnation technique, and are said to enhance reactivity by increasing the catalyst’s Lewis basicity. Herein, however, an alternative method of increasing the basicity of the catalyst is explored by doping nitrogen heteroatoms directly carbon nanotube support structure during synthesis resulting in a novel catalyst referred to as [email protected] This thesis explores the synthesis, characterisation and reactivity of [email protected] to determine the potential for nitrogen doping to enhance the activity of carbon-supported iron nanoparticles in CO2 hydrogenation. The influence of reaction conditions and the addition of synergistic promoter metals are also explored. Nitrogen doping in [email protected] serves to enhance the basicity of the catalyst, resulting in notably increased CO2 conversion and decreased CO selectivity relative to nitrogen-free [email protected] However, methane production also increases as a consequence of nitrogen doping, and a trade-off is observed between CO2 conversion and high α values in the FT product distribution. This unexpected observation is largely attributed to the influence of local C—N dipoles in the catalyst surface upon the adsorption properties of the dipole-containing CO2 and CO reactant molecules and the significantly less polar hydrocarbon products. This behaviour is subsequently exploited further to develop a primarily iron-based, FT-driven methanation catalyst using a significantly lower ruthenium loading than similar catalysts in literature.

Subjects/Keywords: CO2; Catalysis; Fischer-Tropsch; Reverse Water Gas Shift; Water Gas Shift; Carbon Nanotubes; Hydrocarbons

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APA (6^th Edition):

Williamson, D. (2020). Nanostructured catalysts for conversion of CO2 into hydrocarbons. (Doctoral Dissertation). University of Bath. Retrieved from https://researchportal.bath.ac.uk/en/studentthesis/nanostructured-catalysts-for-conversion-of-co2-into-hydrocarbons(60b3567d-d95a-417e-9029-ab06ba68a963).html ; https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.805662

Chicago Manual of Style (16^th Edition):

Williamson, David. “Nanostructured catalysts for conversion of CO2 into hydrocarbons.” 2020. Doctoral Dissertation, University of Bath. Accessed April 17, 2021. https://researchportal.bath.ac.uk/en/studentthesis/nanostructured-catalysts-for-conversion-of-co2-into-hydrocarbons(60b3567d-d95a-417e-9029-ab06ba68a963).html ; https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.805662.

MLA Handbook (7^th Edition):

Williamson, David. “Nanostructured catalysts for conversion of CO2 into hydrocarbons.” 2020. Web. 17 Apr 2021.

Vancouver:

Williamson D. Nanostructured catalysts for conversion of CO2 into hydrocarbons. [Internet] [Doctoral dissertation]. University of Bath; 2020. [cited 2021 Apr 17]. Available from: https://researchportal.bath.ac.uk/en/studentthesis/nanostructured-catalysts-for-conversion-of-co2-into-hydrocarbons(60b3567d-d95a-417e-9029-ab06ba68a963).html ; https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.805662.

Council of Science Editors:

Williamson D. Nanostructured catalysts for conversion of CO2 into hydrocarbons. [Doctoral Dissertation]. University of Bath; 2020. Available from: https://researchportal.bath.ac.uk/en/studentthesis/nanostructured-catalysts-for-conversion-of-co2-into-hydrocarbons(60b3567d-d95a-417e-9029-ab06ba68a963).html ; https://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.805662

Penn State University

2. Kugai, Junichiro. Kinetics of Oxygen-enhanced Water Gas Shift on Bimetallic Catalysts and the Roles of Metals and Support.

Degree: 2011, Penn State University

URL: https://submit-etda.libraries.psu.edu/catalog/11599

► The post-processing of reformate is an important step in producing hydrogen (H2) with low carbon monoxide (CO) for low temperature fuel cells from syn-gas. However,… (more)

▼ The post-processing of reformate is an important step in producing hydrogen (H2) with low carbon monoxide (CO) for low temperature fuel cells from syn-gas. However, the conventional process consists of three steps, i.e. two steps of water gas shift (WGS) and preferential oxidation (PROX) of CO, and it is not suitable for mobile applications due to the large volume of water gas shift (WGS) catalysts and conditioning and/or regeneration necessary for these catalysts. Aiming at replacing those three steps by a simple one-step process, small amount of oxygen was added to WGS (the reaction called oxygen-enhanced water gas shift or OWGS) to promote the reaction kinetics and low pyrophoric ceria-supported bimetallic catalysts were employed for stable performance in this reaction. Not only CO conversion, but also H2 yield was found to increase by the O2 addition on CeO2-supported catalysts. The characteristics of OWGS, high H2 production rate at 200 to 300 °C at short contact time where unreacted O2 exists, evidenced the impact of O2 addition on surface species on the catalyst. Around 1.5 of reaction order in CO for various CeO2-supported metal catalysts for OWGS compared to reaction orders in CO ranging from -0.1 to 0.6 depending on metal species for WGS shows O2 addition decreases CO coverage to free up the active sites for co-reactant (H2O) adsorption and activation. Among the monometallic and bimetallic catalysts, Pt-Cu and Pd-Cu bimetallic catalysts were superior to monometallic catalysts in OWGS. These bimetallic components were found to form alloys where noble metal is surrounded mainly by Cu to have strong interaction between noble metal and copper resulting in high OWGS activity and low pyrophoric property. The metal loadings were optimized for CeO2-supported Pd-Cu bimetallic system and 2 wt% Pd with 5 – 10 wt% Cu were found to be the optimum for the present OWGS condition. In the kinetic study, Pd in Pd-Cu was shown to increase the active sites for H2O dissociation and/or the subsequent reaction with chemisorbed CO as well as Pd keeps Cu in reduced state. Cu was found to keep Pd dispersed, suppress H2 activation on Pd, and facilitate CO2 desorption from catalyst surface. While composition and structure of metal have large impacts on OWGS performance, CeO2 was shown to create new sites for H2O activation at metal-ceria interfacial region in concert with metal. These new sites strongly activate H2O to drive OWGS and WGS compared to the pure metallic sites which are present in majority on Al2O3-supported catalyst. The observed two regimes of turnover rate, the one dependent on catalyst surface area and the other independent of surface area, strongly suggested bifunctional reaction pathway where the reaction rate is determined by activation of H2O and by association of chemisorbed CO and H2O. The associative route was also evidenced by pulse response study where the reaction occurs only when CO and H2O pulses are supplied together, and thus pre-adsorbed species such as formate and carbonate identified by FT-IR are… Advisors/Committee Members: Chunshan Song, Dissertation Advisor/Co-Advisor, Chunshan Song, Committee Chair/Co-Chair, Yaw D Yeboah, Committee Member, Yongsheng Chen, Committee Member, Michael John Janik, Committee Member.

Subjects/Keywords: Oxygen-enhanced Water Gas Shift (OWGS); Water Gas Shift (WGS); Pd; Cu; Metal Catalyst; CeO2-supported Pd-Cu; Bimetallic catalyst

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APA (6^th Edition):

Kugai, J. (2011). Kinetics of Oxygen-enhanced Water Gas Shift on Bimetallic Catalysts and the Roles of Metals and Support. (Thesis). Penn State University. Retrieved from https://submit-etda.libraries.psu.edu/catalog/11599

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Kugai, Junichiro. “Kinetics of Oxygen-enhanced Water Gas Shift on Bimetallic Catalysts and the Roles of Metals and Support.” 2011. Thesis, Penn State University. Accessed April 17, 2021. https://submit-etda.libraries.psu.edu/catalog/11599.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Kugai, Junichiro. “Kinetics of Oxygen-enhanced Water Gas Shift on Bimetallic Catalysts and the Roles of Metals and Support.” 2011. Web. 17 Apr 2021.

Vancouver:

Kugai J. Kinetics of Oxygen-enhanced Water Gas Shift on Bimetallic Catalysts and the Roles of Metals and Support. [Internet] [Thesis]. Penn State University; 2011. [cited 2021 Apr 17]. Available from: https://submit-etda.libraries.psu.edu/catalog/11599.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Kugai J. Kinetics of Oxygen-enhanced Water Gas Shift on Bimetallic Catalysts and the Roles of Metals and Support. [Thesis]. Penn State University; 2011. Available from: https://submit-etda.libraries.psu.edu/catalog/11599

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Mississippi State University

3. Wijayapala, Hevagamage Rangana Thilan. Catalytic conversion of biomass to bio-fuels.

Degree: PhD, Chemistry, 2014, Mississippi State University

URL: http://sun.library.msstate.edu/ETD-db/theses/available/etd-10292014-171413/ ;

► The conversion of biomass to bio-fuel has received considerable attention as a sustainable way to produce energy. As worldwide fossil fuels become depleted these… (more)

▼ The conversion of biomass to bio-fuel has received considerable attention as a sustainable way to produce energy. As worldwide fossil fuels become depleted these efforts grow in importance. The overall strategy is to transform the parent biomass feedstock to increase C-C bonds while reducing oxygen in the final products. A catalytic approach is often used to achieve good yields of transportation grade liquid hydrocarbons from biomass. Development of novel catalyst systems to aid in the thermochemical conversion of biomass to bio-fuel is the focus of this thesis. Gasification of biomass produces synthesis gas (CO and H₂). Synthesis gas can be converted to liquid hydrocarbons using Fischer-Tropsch (FT) synthesis. Mo/ZSM-5 FT catalysts with a potassium (K) promoter are introduced to enhance liquid hydrocarbon production and CO conversion of synthesis gas. Liquid products and CO conversion were determined using GC-MS analysis with respect to changes in K loading from 0-2%. The highest liquid product selectivity (21.7%) was found with 1.0% K loading while largest CO conversion (63%) was found with 1.2% K loading. This catalyst work was extended by introducing Ni and Co into the Mo/ZSM-5 catalysts. A copper based water gas shift catalyst (WGS) was also used in concert with the FT catalyst to improve product selectivity. This WGS catalyst promotes the in-situ production of H2 while decreasing water content. The FT+WGS catalyst were used to convert both 1:1 CO: H₂ syngas and bio-syngas at 280 °C and 350 °C. The liquid hydrocarbon selectivity was significantly changed and the CO conversion was remarkably increased compared to the reactions without the dual catalyst at both temperatures. In the fourth chapter, FT+WGS catalysts were studied for upgrading bio-oil model compounds. Guaiacol and furfural were used as the model compounds and upgrading reactions were done under H₂, syngas and bio-syngas at 200, 250 and 300 °C. Significant conversion of both guaiacol (85%) and furfural (100%) occurred with syngas at 300 °C. Products upgraded from syngas had a higher combined heat of combustion than the products with pure H2. This suggests the incorporation of some C from CO with model compound upgrading reactions with syngas. Advisors/Committee Members: Dr Todd E. Mlsna (chair), Dr. David O. Wipf (committee member), Dr. Dongmao Zhang (committee member), Dr. Svein Saebo (committee member), Dr. Fei Yu (committee member).

Subjects/Keywords: Water gas shift reaction; Biomass to liquid; Heterogeneous catalyst; FischerTropsch synthesis

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APA (6^th Edition):

Wijayapala, H. R. T. (2014). Catalytic conversion of biomass to bio-fuels. (Doctoral Dissertation). Mississippi State University. Retrieved from http://sun.library.msstate.edu/ETD-db/theses/available/etd-10292014-171413/ ;

Chicago Manual of Style (16^th Edition):

Wijayapala, Hevagamage Rangana Thilan. “Catalytic conversion of biomass to bio-fuels.” 2014. Doctoral Dissertation, Mississippi State University. Accessed April 17, 2021. http://sun.library.msstate.edu/ETD-db/theses/available/etd-10292014-171413/ ;.

MLA Handbook (7^th Edition):

Wijayapala, Hevagamage Rangana Thilan. “Catalytic conversion of biomass to bio-fuels.” 2014. Web. 17 Apr 2021.

Vancouver:

Wijayapala HRT. Catalytic conversion of biomass to bio-fuels. [Internet] [Doctoral dissertation]. Mississippi State University; 2014. [cited 2021 Apr 17]. Available from: http://sun.library.msstate.edu/ETD-db/theses/available/etd-10292014-171413/ ;.

Council of Science Editors:

Wijayapala HRT. Catalytic conversion of biomass to bio-fuels. [Doctoral Dissertation]. Mississippi State University; 2014. Available from: http://sun.library.msstate.edu/ETD-db/theses/available/etd-10292014-171413/ ;

4. Wainaina, Steven. Effect of heavy metals on syngas fermentation.

Degree: Engineering and Business, 2016, University of Borås

URL: http://urn.kb.se/resolve?urn=urn:nbn:se:hb:diva-10203

► The goal of this work was to establish the suitable and limiting concentrations of Zn, Cu and Mn compounds during syngas fermentation. The results… (more)

Subjects/Keywords: Syngas biomethanation; biological water-gas-shift; heavy metals

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APA (6^th Edition):

Wainaina, S. (2016). Effect of heavy metals on syngas fermentation. (Thesis). University of Borås. Retrieved from http://urn.kb.se/resolve?urn=urn:nbn:se:hb:diva-10203

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Wainaina, Steven. “Effect of heavy metals on syngas fermentation.” 2016. Thesis, University of Borås. Accessed April 17, 2021. http://urn.kb.se/resolve?urn=urn:nbn:se:hb:diva-10203.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Wainaina, Steven. “Effect of heavy metals on syngas fermentation.” 2016. Web. 17 Apr 2021.

Vancouver:

Wainaina S. Effect of heavy metals on syngas fermentation. [Internet] [Thesis]. University of Borås; 2016. [cited 2021 Apr 17]. Available from: http://urn.kb.se/resolve?urn=urn:nbn:se:hb:diva-10203.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Wainaina S. Effect of heavy metals on syngas fermentation. [Thesis]. University of Borås; 2016. Available from: http://urn.kb.se/resolve?urn=urn:nbn:se:hb:diva-10203

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Delft University of Technology

5. De Lange, M.F. (author). Fricdiff: Parameter estimation and feasibility assessment of combination of Fricdiff and reaction.

Degree: 2010, Delft University of Technology

URL: http://resolver.tudelft.nl/uuid:54fcb117-5167-4738-afbc-f0ede476aafe

►

Fricdiff, which either stands for frictional diffusion or frictional difference is a separation technology for the separation of gas and vapour mixtures. It is based… (more)

Subjects/Keywords: Fricdif; separation; water-gas shift

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APA (6^th Edition):

De Lange, M. F. (. (2010). Fricdiff: Parameter estimation and feasibility assessment of combination of Fricdiff and reaction. (Masters Thesis). Delft University of Technology. Retrieved from http://resolver.tudelft.nl/uuid:54fcb117-5167-4738-afbc-f0ede476aafe

Chicago Manual of Style (16^th Edition):

De Lange, M F (author). “Fricdiff: Parameter estimation and feasibility assessment of combination of Fricdiff and reaction.” 2010. Masters Thesis, Delft University of Technology. Accessed April 17, 2021. http://resolver.tudelft.nl/uuid:54fcb117-5167-4738-afbc-f0ede476aafe.

MLA Handbook (7^th Edition):

De Lange, M F (author). “Fricdiff: Parameter estimation and feasibility assessment of combination of Fricdiff and reaction.” 2010. Web. 17 Apr 2021.

Vancouver:

De Lange MF(. Fricdiff: Parameter estimation and feasibility assessment of combination of Fricdiff and reaction. [Internet] [Masters thesis]. Delft University of Technology; 2010. [cited 2021 Apr 17]. Available from: http://resolver.tudelft.nl/uuid:54fcb117-5167-4738-afbc-f0ede476aafe.

Council of Science Editors:

De Lange MF(. Fricdiff: Parameter estimation and feasibility assessment of combination of Fricdiff and reaction. [Masters Thesis]. Delft University of Technology; 2010. Available from: http://resolver.tudelft.nl/uuid:54fcb117-5167-4738-afbc-f0ede476aafe

University of Notre Dame

6. John Clay. Comparison of Palladium and Platinum Water Gas Shift Kinetics Using Density Functional Theory Models</h1>.

Degree: Chemical and Biomolecular Engineering, 2014, University of Notre Dame

URL: https://curate.nd.edu/show/ks65h992161

► The Water Gas Shift (WGS) reaction can be either thermodynamically or kinetically limited, depending on process conditions. Improved catalysts are of particular interest at… (more)

▼ The Water Gas Shift (WGS) reaction can be either thermodynamically or kinetically limited, depending on process conditions. Improved catalysts are of particular interest at low temperatures where kinetic limitations dominate. In this work, density functional theory calculations were performed to calculate the binding energies, reaction energies, and activation barriers for the proposed WGS pathways on Pt and Pd(111). In addition to the previously published pathways, a new reaction involving the concerted formation of the carboxyl intermediate from water and CO is introduced. In general, binding energies and reaction energies are close on both surfaces. However, Pt has lower activation barriers. Since CO is important for WGS, the CO-CO interactions on Pd(111) were studied by the development of a cluster expansion. A cluster expansion is a polynomial function that allows for rapid prediction of the energy if a structure is given. At low coverages, CO adsorbs in HCP Hollow sites. As the CO coverage increases, CO begins to adsorb in FCC Hollow and Atop sites until the saturation coverage of ¾ ML. Next grand canonical Monte Carlo simulations were performed to determine the coverage-dependent binding energy and temperature programmed desorption spectrum. Finally, a kinetic model was developed to analyze the different WGS reaction pathways, and metals. On both the Pt and Pd surfaces, WGS proceeds through the carboxyl intermediate with water dissociation being the rate determining step, but yields an unfavorably high CO coverage. Next, a coverage dependent binding energy of CO was included in the kinetic model. As the CO binding energy becomes less exothermic, WGS still proceeds through the carboxyl intermediate but carboxyl formation becomes rate determining. Also, the kinetic model shows that Pt is more active than Pd, independent of the CO binding energy. However, the calculated apparent activation barriers and rates do not agree with the experimental results of Pt and Pd supported on Al2O3, which suggest that the support plays an active role in catalyzing the WGS reaction. Since the support plays an important role in WGS catalysis, future studies should attempt to understand the promoting effect of the support and the support-metal interaction. Advisors/Committee Members: W. Nicholas Delgass, Committee Member, Steven Corcelli, Committee Member, William F. Schneider, Committee Chair, Jeffery Kantor, Committee Member.

Subjects/Keywords: Density Functional Theory; Kinetic Modeling; Pt; Pd; Water Gas Shift

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Clay, J. (2014). Comparison of Palladium and Platinum Water Gas Shift Kinetics Using Density Functional Theory Models</h1>. (Thesis). University of Notre Dame. Retrieved from https://curate.nd.edu/show/ks65h992161

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Clay, John. “Comparison of Palladium and Platinum Water Gas Shift Kinetics Using Density Functional Theory Models</h1>.” 2014. Thesis, University of Notre Dame. Accessed April 17, 2021. https://curate.nd.edu/show/ks65h992161.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Clay, John. “Comparison of Palladium and Platinum Water Gas Shift Kinetics Using Density Functional Theory Models</h1>.” 2014. Web. 17 Apr 2021.

Vancouver:

Clay J. Comparison of Palladium and Platinum Water Gas Shift Kinetics Using Density Functional Theory Models</h1>. [Internet] [Thesis]. University of Notre Dame; 2014. [cited 2021 Apr 17]. Available from: https://curate.nd.edu/show/ks65h992161.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Clay J. Comparison of Palladium and Platinum Water Gas Shift Kinetics Using Density Functional Theory Models</h1>. [Thesis]. University of Notre Dame; 2014. Available from: https://curate.nd.edu/show/ks65h992161

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Tennessee – Knoxville

7. Houston, Ross Wesley. Computational Fluid Dynamic Modeling of Catalytic Hydrous Pyrolysis of Biomass to Produce Refinery-Ready Bio-Crude Oil.

Degree: MS, Biosystems Engineering, 2018, University of Tennessee – Knoxville

URL: https://trace.tennessee.edu/utk_gradthes/5122

► The growing world population continually increases the demand for energy. Currently, the main source of energy production is fossil fuels, which are harmful to the… (more)

▼ The growing world population continually increases the demand for energy. Currently, the main source of energy production is fossil fuels, which are harmful to the environment and are finite. An exploration of renewable energy to supplement or replace fossil fuels is of great importance. Modern techniques for producing renewable bio-oil consist of converting biomass into bio-oil through pyrolysis, but unfortunately, pyrolysis oil has quality issues (e.g., high oxygen content, viscosity, chemical instability). Therefore, upgrading is necessary to improve quality. Hydropyrolysis is a state of the art technique to deoxygenate bio-oil during pyrolysis to produce petroleum quality bio-oil. A major issue with hydropyrolysis is the expensive cost of hydrogen.This project aimed to computationally model the hydrous pyrolysis of biomass coupled with an <i>in-situ</i> hydrogen generation process. The kinetics of the water-gas shift (WGS) were determined experimentally and modeled using an ordinary differential equation subroutine coupled with a nonlinear regression. A computational fluid dynamic (CFD) model of biomass fast pyrolysis was developed to simulate conventional fast pyrolysis. The final part of this project adapted the CFD model to simulate hydrous pyrolysis and incorporate the determined WGS kinetics. The bio-oil was deoxygenated via a global lumped hydrodeoxygenation (HDO) kinetic scheme.This WGS was determined to have an agreement with both an empirical power law and a Langmuir-Hinselwood mechanism at conditions similar to that of pyrolysis. The CO conversion reached a maximum value of 94% at higher temps and larger amounts of catalyst. The CFD model of fast pyrolysis predicted a maximum bio-oil yield of 47%, but significantly under-predicted the amount of water present in the oil. The hydrous pyrolysis simulations have not yet reached steady-state and the HDO reactions are just beginning to take place. Further work is needed to explore more detailed kinetic schemes for the secondary pyrolysis reactions as well as the hydrodeoxygenation kinetics. Advisors/Committee Members: Nourredine H. Abdoulmoumine, Douglas G. Hayes, Nicole Labbe.

Subjects/Keywords: Biomass; bio-oil; computational fluid dynamics; hydrous pyrolysis; water gas shift

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Houston, R. W. (2018). Computational Fluid Dynamic Modeling of Catalytic Hydrous Pyrolysis of Biomass to Produce Refinery-Ready Bio-Crude Oil. (Thesis). University of Tennessee – Knoxville. Retrieved from https://trace.tennessee.edu/utk_gradthes/5122

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Houston, Ross Wesley. “Computational Fluid Dynamic Modeling of Catalytic Hydrous Pyrolysis of Biomass to Produce Refinery-Ready Bio-Crude Oil.” 2018. Thesis, University of Tennessee – Knoxville. Accessed April 17, 2021. https://trace.tennessee.edu/utk_gradthes/5122.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Houston, Ross Wesley. “Computational Fluid Dynamic Modeling of Catalytic Hydrous Pyrolysis of Biomass to Produce Refinery-Ready Bio-Crude Oil.” 2018. Web. 17 Apr 2021.

Vancouver:

Houston RW. Computational Fluid Dynamic Modeling of Catalytic Hydrous Pyrolysis of Biomass to Produce Refinery-Ready Bio-Crude Oil. [Internet] [Thesis]. University of Tennessee – Knoxville; 2018. [cited 2021 Apr 17]. Available from: https://trace.tennessee.edu/utk_gradthes/5122.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Houston RW. Computational Fluid Dynamic Modeling of Catalytic Hydrous Pyrolysis of Biomass to Produce Refinery-Ready Bio-Crude Oil. [Thesis]. University of Tennessee – Knoxville; 2018. Available from: https://trace.tennessee.edu/utk_gradthes/5122

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Purdue University

8. Mehta, Dhairya Dilip. Kinetic Studies of Model Reactions to Transform Biomass into Fuels.

Degree: PhD, Chemical Engineering, 2014, Purdue University

URL: https://docs.lib.purdue.edu/open_access_dissertations/1066

► Second-generation biofuels utilizing lignocellulosic biomass are considered to be a promising alternative to fossil-based fuels. Lignocellulosic biomass is structurally diverse and therefore requires detailed understanding… (more)

Subjects/Keywords: Catalysis; Hydrodeoxygenation; Hydropyrolysis; Kinetics; liquid water gas shift; Pt bimetallic

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Mehta, D. D. (2014). Kinetic Studies of Model Reactions to Transform Biomass into Fuels. (Doctoral Dissertation). Purdue University. Retrieved from https://docs.lib.purdue.edu/open_access_dissertations/1066

Chicago Manual of Style (16^th Edition):

Mehta, Dhairya Dilip. “Kinetic Studies of Model Reactions to Transform Biomass into Fuels.” 2014. Doctoral Dissertation, Purdue University. Accessed April 17, 2021. https://docs.lib.purdue.edu/open_access_dissertations/1066.

MLA Handbook (7^th Edition):

Mehta, Dhairya Dilip. “Kinetic Studies of Model Reactions to Transform Biomass into Fuels.” 2014. Web. 17 Apr 2021.

Vancouver:

Mehta DD. Kinetic Studies of Model Reactions to Transform Biomass into Fuels. [Internet] [Doctoral dissertation]. Purdue University; 2014. [cited 2021 Apr 17]. Available from: https://docs.lib.purdue.edu/open_access_dissertations/1066.

Council of Science Editors:

Mehta DD. Kinetic Studies of Model Reactions to Transform Biomass into Fuels. [Doctoral Dissertation]. Purdue University; 2014. Available from: https://docs.lib.purdue.edu/open_access_dissertations/1066

Purdue University

9. Mehta, Dhairya Dilip. Kinetic Studies of Model Reactions to Transform Biomass into Fuels.

Degree: PhD, Chemical Engineering, 2014, Purdue University

URL: https://docs.lib.purdue.edu/open_access_dissertations/1057

► Second-generation biofuels utilizing lignocellulosic biomass are considered to be a promising alternative to fossil-based fuels. Lignocellulosic biomass is structurally diverse and therefore requires detailed… (more)

Subjects/Keywords: Catalysis; Hydrodeoxygenation; Hydropyrolysis; Kinetics; liquid water gas shift; Pt bimetallic

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Mehta, D. D. (2014). Kinetic Studies of Model Reactions to Transform Biomass into Fuels. (Doctoral Dissertation). Purdue University. Retrieved from https://docs.lib.purdue.edu/open_access_dissertations/1057

Chicago Manual of Style (16^th Edition):

Mehta, Dhairya Dilip. “Kinetic Studies of Model Reactions to Transform Biomass into Fuels.” 2014. Doctoral Dissertation, Purdue University. Accessed April 17, 2021. https://docs.lib.purdue.edu/open_access_dissertations/1057.

MLA Handbook (7^th Edition):

Mehta, Dhairya Dilip. “Kinetic Studies of Model Reactions to Transform Biomass into Fuels.” 2014. Web. 17 Apr 2021.

Vancouver:

Mehta DD. Kinetic Studies of Model Reactions to Transform Biomass into Fuels. [Internet] [Doctoral dissertation]. Purdue University; 2014. [cited 2021 Apr 17]. Available from: https://docs.lib.purdue.edu/open_access_dissertations/1057.

Council of Science Editors:

Mehta DD. Kinetic Studies of Model Reactions to Transform Biomass into Fuels. [Doctoral Dissertation]. Purdue University; 2014. Available from: https://docs.lib.purdue.edu/open_access_dissertations/1057

The Ohio State University

10. Gawade, Preshit Vilas. REDOX CATALYSIS FOR ENVIRONMENTAL APPLICATIONS.

Degree: PhD, Chemical and Biomolecular Engineering, 2012, The Ohio State University

URL: http://rave.ohiolink.edu/etdc/view?acc_num=osu1341412462

► The presented work comprehends a broad spectrum of redox catalysis for various environmental applications, such as i) hydrogen production via water-gas shift reaction, ii)… (more)

▼ The presented work comprehends a broad spectrum of redox catalysis for various environmental applications, such as i) hydrogen production via water-gas shift reaction, ii) hydrogen purification for fuel cell applications and iii) catalytic after-treatment of lean-burn engines. This dissertation involves, but is not limited to catalyst development, reaction studies and catalyst characterization for the above-mentioned environmental applications, which can be summarized as follows. (i) Water-gas shift (WGS) remains an essential step in integrated gasification combined cycle (IGCC) for hydrogen production, as it forms a link between the gasification process and fuel cell operations. The current catalysts for WGS application are based on Fe-Cr and Cu/ZnO/Al2O3, as a high temperature (HT-WGS) and low temperature (LT-WGS) catalysts, respectively. This two-stage WGS process is a consequence of several operational drawbacks of the current catalyst formulations including Cr+6 being carcinogenic. Hence the presented WGS project has a two-fold purpose. First, Cr-free Fe-based catalyst development and second, Cu supported catalyst development for WGS that can be operated over a wide temperature range. In this dissertation, Cr- free Fe-Al-Cu catalyst prepared through “one-step” sol-gel method using propylene oxide as a gelation agent has been reported. Steady state reactions demonstrated that WGS performance of Fe-Al-Cu was superior as compared to commercial Fe-Cr catalyst. The reaction studies along with complementary catalyst characterization indicated that the amount of copper in iron oxide matrix played a crucial role. The optimized ratio of Fe to Cu was found to be five and any further increase in copper loading resulted in copper segregation from the iron oxide matrix. Thus various catalyst characterization techniques were exploited to understand this phenomenon. Furthermore, a detailed study was performed to comprehend the formation of surface species during WGS reaction and to evaluate the reaction mechanism over Fe-Al-Cu. In the quest of exploring Cu-based catalyst for WGS system, Cu supported over various CeO2 nano-morphologies were investigated. Here, nanoparticles (NP) and nanorods (NR) of CeO2 were prepared through hydrothermal precipitation method and copper was supported on these morphologies using a wet impregnation method. In the current findings, copper was more finely and uniformly dispersed over CeO2 nano-particles compared to nanorods, resulting in better WGS activity compared to particle-based samples. Catalyst characterization indicated finely dispersed copper particles in close interaction with ceria nanoparticles, whereas isolated bulk-like copper species were formed over the ceria nanorods. Finally, the formation of surface species during WGS reaction delineated the redox reaction mechanism over Cu/CeO2. (ii) Hydrogen produced via WGS reaction may contain up to 1-2% CO in stream which can be poisonous to proton exchange membrane (PEM) fuel cell. Preferential oxidation of… Advisors/Committee Members: Ozkan, Umit (Advisor).

Subjects/Keywords: Chemical Engineering; Water-gas-shift; PROX; hydrocarbon-SCR; catalyst; emission

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Gawade, P. V. (2012). REDOX CATALYSIS FOR ENVIRONMENTAL APPLICATIONS. (Doctoral Dissertation). The Ohio State University. Retrieved from http://rave.ohiolink.edu/etdc/view?acc_num=osu1341412462

Chicago Manual of Style (16^th Edition):

Gawade, Preshit Vilas. “REDOX CATALYSIS FOR ENVIRONMENTAL APPLICATIONS.” 2012. Doctoral Dissertation, The Ohio State University. Accessed April 17, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=osu1341412462.

MLA Handbook (7^th Edition):

Gawade, Preshit Vilas. “REDOX CATALYSIS FOR ENVIRONMENTAL APPLICATIONS.” 2012. Web. 17 Apr 2021.

Vancouver:

Gawade PV. REDOX CATALYSIS FOR ENVIRONMENTAL APPLICATIONS. [Internet] [Doctoral dissertation]. The Ohio State University; 2012. [cited 2021 Apr 17]. Available from: http://rave.ohiolink.edu/etdc/view?acc_num=osu1341412462.

Council of Science Editors:

Gawade PV. REDOX CATALYSIS FOR ENVIRONMENTAL APPLICATIONS. [Doctoral Dissertation]. The Ohio State University; 2012. Available from: http://rave.ohiolink.edu/etdc/view?acc_num=osu1341412462

11. Huve, Joffrey. Highly selective, active and stable Fischer-Tropsch catalyst using entrapped iron nanoparticles in silicalite-1 : Catalyseur de Fischer-Tropsch hautement sélectif, actif et stable utilisant des nanoparticules de fer encapsulées dans une zéolithe de type Silicalite-1.

Degree: Docteur es, Chimie, 2017, Lyon

URL: http://www.theses.fr/2017LYSE1042

►

L'intérêt pour la synthèse de Fischer-Tropsch (FTS) est d'actualité. Elle permet la conversion de matière première (biomasse) en combustible liquide. Comparés aux catalyseurs à base… (more)

▼

L'intérêt pour la synthèse de Fischer-Tropsch (FTS) est d'actualité. Elle permet la conversion de matière première (biomasse) en combustible liquide. Comparés aux catalyseurs à base de cobalt, ceux à base de fer présentent une désactivation rapide, une activité et une sélectivité faibles en produisant une quantité non désirable de CO2. Après plusieurs décennies d'études, l'origine de ces défauts reste méconnue. Les catalyseurs classiques sont généralement fortement chargés en fer (>70 wt.%) et composés de nombreuses phases empêchant l'établissement d'une relation structure-activité. Il est nécessaire de développer des catalyseurs contenant du fer plus actifs, plus sélectifs et plus stables par une approche rationnelle. La synthèse de nanoparticules de taille contrôlée (3.5 nm) encapsulées dans les murs d'une silicalite-1 creuse ([email protected]) est présentée. L'encapsulation empêche le frittage pendant la synthèse de Fischer-Tropsch, permettant de garder une bonne dispersion du fer. Contrairement aux autres catalyseurs, le catalyseur [email protected] ne produit pas de CO2. L'hydrophobicité de la silicalite-1 est très certainement à l'origine de la non-production de CO2 par inhibition de la réaction directe du gaz à l'eau. On démontre que le catalyseur [email protected] le CO2 en CO par réaction du gaz à l'eau inversée (R-WGS). Afin d'établir une relation structure-activité, des catalyseurs à base de fer de taille bien contrôlée sont synthétisés et caractérisés (MET, in-situ XANES, in-situ Mössbauer). Deux catégories de TOF suivant la taille des particules, ~10-2 s-1 pour les plus larges (>20 nm) et ~10-3 s-1 pour les plus petites, sont observées

Fischer-Tropsch synthesis (FTS) is gaining renewed interests as it allows converting alternative feedstocks (biomass) into liquid fuels. Compared to Co-based catalysts, state of the art Fe catalysts show lower activity, faster deactivation and lower selectivity as it produces an undesirable amount of CO2. Despite decades of studies, the origins of low activity and selectivity and fast deactivation are still unclear. Typical Fe based catalysts are highly metal loaded (>70 wt.%) and composed of many different phases, which strongly impedes the establishment of structure-activity relationships. There is a need to develop more active, more selective and more stable iron FTS catalysts by rational approaches.The synthesis of well-controlled 3.5 nm iron nanoparticles encapsulated in the walls of a hollow-silicalite-1 zeolite ([email protected]) is presented. The encapsulation prevents particle sintering under FTS conditions leading to a high and stable Fe dispersion. The catalyst [email protected] is active and highly selective in FTS. Most importantly, [email protected] does not produce CO2 in contrast to all other Fe-based catalysts. The strong hydrophobicity of the silicalite-1 is likely the origin of the lack of CO2 production by inhibition of the forward WGS reaction. We demonstrated that [email protected] CO2 into…

Advisors/Committee Members: Farrusseng, David (thesis director), Schuurman, Yves (thesis director).

Subjects/Keywords: Fischer-Tropsch synthesis; Water-gas-shift; Activité; Selectivité; Stabilité; TOF; CO2; Fer; Fischer-Tropsch synthesis; Water-gas-shift; Activity; Selectivity; Stability; TOF; CO2; Iron catalyst; 541.395

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Huve, J. (2017). Highly selective, active and stable Fischer-Tropsch catalyst using entrapped iron nanoparticles in silicalite-1 : Catalyseur de Fischer-Tropsch hautement sélectif, actif et stable utilisant des nanoparticules de fer encapsulées dans une zéolithe de type Silicalite-1. (Doctoral Dissertation). Lyon. Retrieved from http://www.theses.fr/2017LYSE1042

Chicago Manual of Style (16^th Edition):

Huve, Joffrey. “Highly selective, active and stable Fischer-Tropsch catalyst using entrapped iron nanoparticles in silicalite-1 : Catalyseur de Fischer-Tropsch hautement sélectif, actif et stable utilisant des nanoparticules de fer encapsulées dans une zéolithe de type Silicalite-1.” 2017. Doctoral Dissertation, Lyon. Accessed April 17, 2021. http://www.theses.fr/2017LYSE1042.

MLA Handbook (7^th Edition):

Huve, Joffrey. “Highly selective, active and stable Fischer-Tropsch catalyst using entrapped iron nanoparticles in silicalite-1 : Catalyseur de Fischer-Tropsch hautement sélectif, actif et stable utilisant des nanoparticules de fer encapsulées dans une zéolithe de type Silicalite-1.” 2017. Web. 17 Apr 2021.

Vancouver:

Huve J. Highly selective, active and stable Fischer-Tropsch catalyst using entrapped iron nanoparticles in silicalite-1 : Catalyseur de Fischer-Tropsch hautement sélectif, actif et stable utilisant des nanoparticules de fer encapsulées dans une zéolithe de type Silicalite-1. [Internet] [Doctoral dissertation]. Lyon; 2017. [cited 2021 Apr 17]. Available from: http://www.theses.fr/2017LYSE1042.

Council of Science Editors:

Huve J. Highly selective, active and stable Fischer-Tropsch catalyst using entrapped iron nanoparticles in silicalite-1 : Catalyseur de Fischer-Tropsch hautement sélectif, actif et stable utilisant des nanoparticules de fer encapsulées dans une zéolithe de type Silicalite-1. [Doctoral Dissertation]. Lyon; 2017. Available from: http://www.theses.fr/2017LYSE1042

12. Renata Uema Ribeiro. Nanopartículas de Pt suportadas em Al2O3 e CeO2-Al2O3: síntese e caracterização de catalisadores aplicados à reação de deslocamento gás-água.

Degree: 2011, Universidade Federal de São Carlos

URL: http://www.bdtd.ufscar.br/htdocs/tedeSimplificado//tde_busca/arquivo.php?codArquivo=5114

►

Nanopartículas de Pt foram preparadas seguindo um procedimento adaptado de Song e colaboradores [1], cuja metodologia consistiu na redução química do ácido hexacloroplatinico pelo etilenoglicol… (more)

▼

Nanopartículas de Pt foram preparadas seguindo um procedimento adaptado de Song e colaboradores [1], cuja metodologia consistiu na redução química do ácido hexacloroplatinico pelo etilenoglicol em meio básico, porém utilizando duas razões PVP/Pt = 0,2 e 10. Ambas as razões levaram a nanopartículas de Pt com tamanho similar (2,0 e 2,8 nm) e monodispersas. As soluções coloidais de nanoparticulas de Pt foram incorporada à alumina durante a síntese sol-gel e mostraram diferentes estabilidades quando submetidas a tratamentos térmicos em ar sintético, He e H2. A razão PVP/Pt utilizada na síntese das partículas foi o fator determinante na estabilidade das partículas no suporte. A adição de uma menor razão PVP/Pt levou a aglomeração das partículas durante a calcinação em ar sintético. Por outro lado, quando um excesso de PVP foi utilizado durante a síntese das partículas as mesmas se mostraram estáveis e dispersas no suporte quando submetidas ao mais severo tratamento. Isto foi relacionado ao ancoramento das partículas ao suporte durante a etapa de incorporação. Nanocatalisadores de Pt suportados em alumina e cério-alumina apresentaram atividade catalítica para a reação de deslocamento gás-água. Dados de conversão do CO indicaram que o aumento no teor de CeO2 de 12 para 20% levou a um aumento na atividade catalítica. Medidas de XPS após a etapa de pré-tratamento em H2 confirmaram a presença de Pt+na superfície dos catalisadores contendo ceria, sugerindo alguma interação metal-suporte. Técnicas de caracterização in situ possibilitaram um melhor entendimento do mecanismo das espécies envolvidas no mecanismo da reação de deslocamento gás-água. Medidas de XANES in situ na borda da Pt confirmaram a presença de Pt reduzida durante o curso da reação para todos os catalisadores, o que sugere a presença de sítios de Pt com densidade eletrônica similar. Isto também foi observado nas medidas de DRIFTS do CO adsorvido para os catalisadores estudados. No entanto, os espectros de XANES na borda do Ce confirmaram mudanças no estado de oxidação do Ce no decorrer da reação, indicando a ocorrência do mecanismo de reação redox, mediado pela ceria. Experimentos utilizando DRIFTS in situ identificaram pequenas concentrações de espécies do tipo formiatos e carbonatos na superfície dos catalisadores durante a reação, sugerindo que mais de um mecanismo pode ocorrer simultaneamente. Palavras chave: nanoparticulas, Platina, catalisador, reação de deslocamento gás-água, PVP.

Colloidal Pt nanoparticles were synthesized according to an adapted procedure from Song and co-workers [1], which it was based on the reduction of dihydrogen hexachloroplatinate by ethylene glycol in a basic solution, but using two PVP/Pt = 0,2 and 10 ratio. Both the ratio lead to monodisperse platinum nanoparticles with similar sizes (2.0 and 2.8 nm). Colloidal Pt nanoparticles solutions were incorporated into alumina during sol-gel synthesis and showed different stabilities when submitted to thermal treatment in synthetic air, He and H2 atmospheres. PVP/Pt…

Advisors/Committee Members: José Maria Corrêa Bueno.

Subjects/Keywords: ENGENHARIA QUIMICA; Catálise; Nanopartículas; Platina; Catalisadores; Nanoparticles; Platinum; Catalyst; Water gas shift reacion; PVP

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Ribeiro, R. U. (2011). Nanopartículas de Pt suportadas em Al2O3 e CeO2-Al2O3: síntese e caracterização de catalisadores aplicados à reação de deslocamento gás-água. (Thesis). Universidade Federal de São Carlos. Retrieved from http://www.bdtd.ufscar.br/htdocs/tedeSimplificado//tde_busca/arquivo.php?codArquivo=5114

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Ribeiro, Renata Uema. “Nanopartículas de Pt suportadas em Al2O3 e CeO2-Al2O3: síntese e caracterização de catalisadores aplicados à reação de deslocamento gás-água.” 2011. Thesis, Universidade Federal de São Carlos. Accessed April 17, 2021. http://www.bdtd.ufscar.br/htdocs/tedeSimplificado//tde_busca/arquivo.php?codArquivo=5114.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Ribeiro, Renata Uema. “Nanopartículas de Pt suportadas em Al2O3 e CeO2-Al2O3: síntese e caracterização de catalisadores aplicados à reação de deslocamento gás-água.” 2011. Web. 17 Apr 2021.

Vancouver:

Ribeiro RU. Nanopartículas de Pt suportadas em Al2O3 e CeO2-Al2O3: síntese e caracterização de catalisadores aplicados à reação de deslocamento gás-água. [Internet] [Thesis]. Universidade Federal de São Carlos; 2011. [cited 2021 Apr 17]. Available from: http://www.bdtd.ufscar.br/htdocs/tedeSimplificado//tde_busca/arquivo.php?codArquivo=5114.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Ribeiro RU. Nanopartículas de Pt suportadas em Al2O3 e CeO2-Al2O3: síntese e caracterização de catalisadores aplicados à reação de deslocamento gás-água. [Thesis]. Universidade Federal de São Carlos; 2011. Available from: http://www.bdtd.ufscar.br/htdocs/tedeSimplificado//tde_busca/arquivo.php?codArquivo=5114

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Brigham Young University

13. Brown, Jared C. UV Visible Spectra Analysis of High Temperature Water Gas Shift Catalysts Made from Iron, Lanthanum, Copper, and Chromium Oxides.

Degree: MS, 2012, Brigham Young University

URL: https://scholarsarchive.byu.edu/cgi/viewcontent.cgi?article=4221&context=etd

► Hydrogen is a vital component in several different chemical reactions as well as a potential fuel source for the future. The water gas shift (WGS)… (more)

▼ Hydrogen is a vital component in several different chemical reactions as well as a potential fuel source for the future. The water gas shift (WGS) reaction converts CO and water to hydrogen and CO2. The objective of this work is to first, characterize the potential benefits of the addition of lanthanum oxide (lanthana) to the iron-chromium-copper (Fe-Cr-Cu) oxide catalysts industrially used in high temperature water gas shift processes, and second, analyze these catalysts using in-situ UV-Visible spectroscopy. The benefits of each component in the catalyst are discussed as well as potential benefits from the addition of lanthana. Lanthana is a rare earth oxide that dramatically increases the surface area of the iron based WGS catalysts, and small concentrations of other rare earth oxides (i.e. cerium) have been shown to increase the rate of desorption of CO2 from iron surfaces (Hu Yanping 2002). Lanthana has similar chemical properties to other rare earth oxides tested and has not been previously tested as an additive to the WGS catalyst. Therefore catalysts with 0, 1, 2, 5, 10, and 20 wt% lanthana were made via a co-precipitation method in order to measure changes in activity, physical stability, and thermal stability. Catalyst characterization techniques utilized include electron dispersive X-ray spectroscopy (EDX), temperature programmed reduction (TPR) with hydrogen, and nitrogen physisorption (BET). The kinetic analysis was performed utilizing both mass spectroscopy (MS) and gas chromatography (GC). The addition of 1 wt% lanthana to the Fe-Cr-Cu catalysts increases WGS reaction rates of the catalyst at 425°C and 350°C, however the 0% La catalyst has the highest rates at 375°C and 400°C. The 0% La catalyst shows significant drop off in rate at 425°C, suggesting that the lanthana provides a small thermal stabilizing, i.e. the addition of lanthana prevents catalyst sintering at higher temperatures. Traditionally, chromia acts as the sole thermal stabilizer in these catalysts. The addition of large amounts of lanthana inhibits the chromia stabilizing effect, however small additions of lanthana appear to have an additional catalyst promotional effect without interfering with the chromia thermal stabilization. The increased WGS reaction rates at higher temperatures could allow for greater throughput of reactants in industrial settings. Higher concentrations of lanthana decrease the activity due to what is believed to be disruption of the chromia stabilizing effect as well as reduced amount of the active phase of catalyst. In-situ UV-Visible analysis shows that the oxidation state of the iron in the catalyst has a direct correlation to the UV-Visible light absorbance of the surface of the iron catalyst. Extent of reduction is traditionally measured with a synchrotron which is significantly more expensive than UV-Vis spectroscopy. This study uses the more economical UV-Vis spectrometer to determine similar information. The lanthana doped catalysts show an over-reduction of iron during WGS conditions (i.e. rapid…

Subjects/Keywords: extent of reduction; water gas shift; lanthana; UV-visible spectroscopy; Chemical Engineering

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APA (6^th Edition):

Brown, J. C. (2012). UV Visible Spectra Analysis of High Temperature Water Gas Shift Catalysts Made from Iron, Lanthanum, Copper, and Chromium Oxides. (Masters Thesis). Brigham Young University. Retrieved from https://scholarsarchive.byu.edu/cgi/viewcontent.cgi?article=4221&context=etd

Chicago Manual of Style (16^th Edition):

Brown, Jared C. “UV Visible Spectra Analysis of High Temperature Water Gas Shift Catalysts Made from Iron, Lanthanum, Copper, and Chromium Oxides.” 2012. Masters Thesis, Brigham Young University. Accessed April 17, 2021. https://scholarsarchive.byu.edu/cgi/viewcontent.cgi?article=4221&context=etd.

MLA Handbook (7^th Edition):

Brown, Jared C. “UV Visible Spectra Analysis of High Temperature Water Gas Shift Catalysts Made from Iron, Lanthanum, Copper, and Chromium Oxides.” 2012. Web. 17 Apr 2021.

Vancouver:

Brown JC. UV Visible Spectra Analysis of High Temperature Water Gas Shift Catalysts Made from Iron, Lanthanum, Copper, and Chromium Oxides. [Internet] [Masters thesis]. Brigham Young University; 2012. [cited 2021 Apr 17]. Available from: https://scholarsarchive.byu.edu/cgi/viewcontent.cgi?article=4221&context=etd.

Council of Science Editors:

Brown JC. UV Visible Spectra Analysis of High Temperature Water Gas Shift Catalysts Made from Iron, Lanthanum, Copper, and Chromium Oxides. [Masters Thesis]. Brigham Young University; 2012. Available from: https://scholarsarchive.byu.edu/cgi/viewcontent.cgi?article=4221&context=etd

University of Ottawa

14. Lortie, Maxime. Reverse Water Gas Shift Reaction over Supported Cu-Ni Nanoparticle Catalysts .

Degree: 2014, University of Ottawa

URL: http://hdl.handle.net/10393/31733

► CuNi nanoparticles were synthesized using a new polyol synthesis method. Three different CuxNi1-x catalysts were synthesized where x = 20, 50 and 80. The nanoparticles… (more)

Subjects/Keywords: Reverse Water Gas Shift; Catalysis; Nanoparticle; Copper Nickel Alloy; Oxygen Vacancy; Samarium-Doped Ceria

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Lortie, M. (2014). Reverse Water Gas Shift Reaction over Supported Cu-Ni Nanoparticle Catalysts . (Thesis). University of Ottawa. Retrieved from http://hdl.handle.net/10393/31733

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Lortie, Maxime. “Reverse Water Gas Shift Reaction over Supported Cu-Ni Nanoparticle Catalysts .” 2014. Thesis, University of Ottawa. Accessed April 17, 2021. http://hdl.handle.net/10393/31733.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Lortie, Maxime. “Reverse Water Gas Shift Reaction over Supported Cu-Ni Nanoparticle Catalysts .” 2014. Web. 17 Apr 2021.

Vancouver:

Lortie M. Reverse Water Gas Shift Reaction over Supported Cu-Ni Nanoparticle Catalysts . [Internet] [Thesis]. University of Ottawa; 2014. [cited 2021 Apr 17]. Available from: http://hdl.handle.net/10393/31733.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Lortie M. Reverse Water Gas Shift Reaction over Supported Cu-Ni Nanoparticle Catalysts . [Thesis]. University of Ottawa; 2014. Available from: http://hdl.handle.net/10393/31733

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Ottawa

15. Wilson, Sean M. W. Adsorption Separation of CO2 from CO in Syngas: Improving the Conversion of the Reverse Water Gas Shift Reaction .

Degree: 2015, University of Ottawa

URL: http://hdl.handle.net/10393/33169

► In this research project, adsorption is considered for the separation of CO2 from CO for applications such as industrial syngas production and in particular to… (more)

▼ In this research project, adsorption is considered for the separation of CO2 from CO for applications such as industrial syngas production and in particular to improve the conversion of the Reverse Water Gas Shift (RWGS) process. The use of adsorption technology for these applications requires an adsorbent that can effectively separate out CO2 from a gas mixture containing CO2, CO, and H2. However, adsorption of H2 is insignificant when compared to both CO2 and CO, with only CO2 and CO being the adsorbed species. The adsorption of CO2 and CO was investigated in this work for four major types of industrial adsorbents which include: activated aluminas, activated carbons, silica gels, and zeolites. Zeolites, with their ability to be fine tuned many parameters which may affect adsorption, were investigated in terms of the effect of the cations present, SiO2/Al2O3 ratios, and structure to determine how to optimize adsorption of CO2 while decreasing adsorption of CO. This will help to determine a promising adsorbent for this separation with focus on maximizing the selective adsorption of CO2 over CO. To investigate this separation three scientific experimental methods were used; gravimetric adsorption isotherm analysis, volumetric adsorption isotherm analysis, and packed bed adsorption desorption breakthrough analysis. Gravimetric and volumetric methods allow for testing the adsorbent with the individual species of CO2 and CO. This investigation will let us determine the pure component adsorption capacity, heats of adsorption, regenerability, and basic selectivity. Packed bed adsorption breakthrough experimentation was then carried out on promising adsorbents for the CO2 separation from a mixture of CO2, CO, and H2. These experiments used a gas mixture that would be comparable to that produced from the RWGS reaction to determine the multicomponent gas mixture behaviour for adsorption. Temperature swing adsorption (TSA) with a purge gas stream of H2 was then used to regenerate the adsorbent.

Subjects/Keywords: Carbon Dioxide and Carbon Monoxide Separation; Adsorption; Reverse Water Gas Shift; Syngas

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Wilson, S. M. W. (2015). Adsorption Separation of CO2 from CO in Syngas: Improving the Conversion of the Reverse Water Gas Shift Reaction . (Thesis). University of Ottawa. Retrieved from http://hdl.handle.net/10393/33169

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Wilson, Sean M W. “Adsorption Separation of CO2 from CO in Syngas: Improving the Conversion of the Reverse Water Gas Shift Reaction .” 2015. Thesis, University of Ottawa. Accessed April 17, 2021. http://hdl.handle.net/10393/33169.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Wilson, Sean M W. “Adsorption Separation of CO2 from CO in Syngas: Improving the Conversion of the Reverse Water Gas Shift Reaction .” 2015. Web. 17 Apr 2021.

Vancouver:

Wilson SMW. Adsorption Separation of CO2 from CO in Syngas: Improving the Conversion of the Reverse Water Gas Shift Reaction . [Internet] [Thesis]. University of Ottawa; 2015. [cited 2021 Apr 17]. Available from: http://hdl.handle.net/10393/33169.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Wilson SMW. Adsorption Separation of CO2 from CO in Syngas: Improving the Conversion of the Reverse Water Gas Shift Reaction . [Thesis]. University of Ottawa; 2015. Available from: http://hdl.handle.net/10393/33169

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Toronto

16. Jelle, Abdinoor Abdullahi. Photochemical and Photothermal Reduction of Carbon Dioxide for Solar Fuels Production.

Degree: PhD, 2017, University of Toronto

URL: http://hdl.handle.net/1807/80970

► Abstract Catalytic conversion of greenhouse gas carbon dioxide to value-added chemicals and fuels powered by solar energy is envisioned to be a promising strategy to… (more)

▼ Abstract Catalytic conversion of greenhouse gas carbon dioxide to value-added chemicals and fuels powered by solar energy is envisioned to be a promising strategy to realize both energy security and environmental protection. This work demonstrates that earth abundant, low cost nanomaterials based on silicon and iron can be used to harvest both light and heat energy from the sun to reduce CO2 and generate solar fuels. Herein, we have demonstrated that ruthenium supported ultra-black silicon nanowires can drive the Sabatier reaction both photochemically and photothermally where both incident photons absorbed by and heat generated in the black silicon nanowires accelerate the photomethanation reaction. This allows the reaction to be activated at ambient temperatures removing the need for external heating that could cause sintering, mechanical degradation and eventual catalyst deactivation and therefore improves the overall energy efficiency of the process. Additionally, we have shown that the rate of photomethanation is greatly enhanced when highly dispersed nanocrystalline RuO2 is chemically deposited onto the black silicon nanowires support. Furthermore, we have demonstrated that other silicon structures such as three-dimensional silicon photonic crystals can be used as an efficient support for CO2 hydrogenation. Unlike other insulating supports, these silicon nanostructured supports are particularly attractive for solar-powered catalysis because, with a band-gap of 1.1 eV, they can potentially absorb 80% of the solar irradiance. Moreover, they exhibit excellent absorption strengths and low reflective losses across the entire solar spectral wavelength range of the ultraviolet, visible and near-infrared portion of the solar spectrum. Finally, we demonstrated a comprehensive comparative study of the physical, electronic, and photocatalytic properties of ironoxyhydroxide (FeOOH) polymorphs by studying the extent of methylene blue photodegradation. This work led to the transformation of these FeOOH polymorphs into magnetite (Fe3O4) which effectively reduced CO2 to CO via the reverse water gas shift (RWGS) reaction. Advisors/Committee Members: Perovic, Doug D., Ozin, Geoffrey A., Materials Science and Engineering.

Subjects/Keywords: Catalysis; Photochemical; Photomethanation; Photothermal; Reverse Water Gas Shift Reaction; Solar Fuels; 0794

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Jelle, A. A. (2017). Photochemical and Photothermal Reduction of Carbon Dioxide for Solar Fuels Production. (Doctoral Dissertation). University of Toronto. Retrieved from http://hdl.handle.net/1807/80970

Chicago Manual of Style (16^th Edition):

Jelle, Abdinoor Abdullahi. “Photochemical and Photothermal Reduction of Carbon Dioxide for Solar Fuels Production.” 2017. Doctoral Dissertation, University of Toronto. Accessed April 17, 2021. http://hdl.handle.net/1807/80970.

MLA Handbook (7^th Edition):

Jelle, Abdinoor Abdullahi. “Photochemical and Photothermal Reduction of Carbon Dioxide for Solar Fuels Production.” 2017. Web. 17 Apr 2021.

Vancouver:

Jelle AA. Photochemical and Photothermal Reduction of Carbon Dioxide for Solar Fuels Production. [Internet] [Doctoral dissertation]. University of Toronto; 2017. [cited 2021 Apr 17]. Available from: http://hdl.handle.net/1807/80970.

Council of Science Editors:

Jelle AA. Photochemical and Photothermal Reduction of Carbon Dioxide for Solar Fuels Production. [Doctoral Dissertation]. University of Toronto; 2017. Available from: http://hdl.handle.net/1807/80970

University of Southern California

17. Abdollahi, Mitra. An integrated 'one-box' process for hydrogen production.

Degree: PhD, Chemical Engineering, 2011, University of Southern California

URL: http://digitallibrary.usc.edu/cdm/compoundobject/collection/p15799coll127/id/471342/rec/768

► Hydrogen is widely considered as a fuel for the future to address the energy crisis and the environmental concerns. In this study, process intensification in… (more)

▼ Hydrogen is widely considered as a fuel for the future to address the energy crisis and the environmental concerns. In this study, process intensification in hydrogen production from natural gas, coal- and biomass-derived syngas is investigated both experimentally and theoretically. A novel reactor/separator system, termed the “one-box” process is being employed. The heart of this system is a membrane reactor (MR) that combines the water-gas shift (WGS) reaction with hydrogen separation into a single unit, thus eliminating the need for the commonly utilized two separate WGS reactors and a distinct purification unit.; Impurity-resistant carbon molecular sieve (CMS) membranes and sour-gas shift catalysts are utilized in order to treat the gas streams with simulated coal/biomass-derived syngas compositions. Both have shown high tolerance for H2S and NH3, which are the main impurities in the syngas (in fact, the sour-gas shift catalysts require sulfur to be present in order to remain active). This adds another benefit to the system by eliminating the need for gas clean-up upstream of the WGS reactor, which saves energy, and significantly simplifies the process design. The CMS membrane stability is further investigated in the presence of model tar and organic vapor compounds. The membranes proved to be stable at temperatures akin to the WGS environment. Permeation loss occurred at lower temperatures; however, regeneration was readily achieved by purging the membranes with inert gas at higher temperatures. This indicates that at low temperatures only surface coverage through condensation occurs, with little or no irreversible pore plugging of the membrane.; The project focus has been on experimental investigations in order to prove the feasibility of using the ‘one-box’ system for H2 production and to validate a mathematical model developed for use for scale-up investigations. Prior to their use in the MR experiments, the membranes are characterized via single and multi-component gas permeation measurements. Packed-bed experiments are also performed in order to derive the kinetic rate expressions. The effect of different experimental conditions on MR performance, in terms of CO conversion, hydrogen product recovery and purity is experimentally studied, and the results are compared with those from the mathematical model. The model is further used for process scale-up, and in order predict the MR performance under conditions akin to the industrial applications. It is shown that the MR-based systems are capable of converting more CO into H2 when compared to the more traditional packed-bed reactors, in some cases attaining almost complete CO conversions.; In addition to the CMS membrane-based MR, we have also investigated palladium (Pd) membranes with infinite selectivity towards hydrogen, combined with low-temperature shift (LTS) catalysts are used for ultra pure hydrogen production from gas streams with simulated natural gas reformate compositions, to serve as a feed for fuel cell applications. One key advantage of using the… Advisors/Committee Members: Tsotsis, Theodore T. (Committee Chair), Sahimi, Muhammad (Committee Member), Pirbazari, Massoud M. (Committee Member).

Subjects/Keywords: hydrogen production; membrane reactor; water-gas shift reaction; carbon membrane; palladium membrane

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APA (6^th Edition):

Abdollahi, M. (2011). An integrated 'one-box' process for hydrogen production. (Doctoral Dissertation). University of Southern California. Retrieved from http://digitallibrary.usc.edu/cdm/compoundobject/collection/p15799coll127/id/471342/rec/768

Chicago Manual of Style (16^th Edition):

Abdollahi, Mitra. “An integrated 'one-box' process for hydrogen production.” 2011. Doctoral Dissertation, University of Southern California. Accessed April 17, 2021. http://digitallibrary.usc.edu/cdm/compoundobject/collection/p15799coll127/id/471342/rec/768.

MLA Handbook (7^th Edition):

Abdollahi, Mitra. “An integrated 'one-box' process for hydrogen production.” 2011. Web. 17 Apr 2021.

Vancouver:

Abdollahi M. An integrated 'one-box' process for hydrogen production. [Internet] [Doctoral dissertation]. University of Southern California; 2011. [cited 2021 Apr 17]. Available from: http://digitallibrary.usc.edu/cdm/compoundobject/collection/p15799coll127/id/471342/rec/768.

Council of Science Editors:

Abdollahi M. An integrated 'one-box' process for hydrogen production. [Doctoral Dissertation]. University of Southern California; 2011. Available from: http://digitallibrary.usc.edu/cdm/compoundobject/collection/p15799coll127/id/471342/rec/768

University of South Florida

18. Ramos, Adela E. Enhanced CO₂ Conversion by the Simultaneous Doping of Co, Fe, and Mn in the B-site of a Lanthanum Perovskite.

Degree: 2018, University of South Florida

URL: https://scholarcommons.usf.edu/etd/8138

► There is a pressing need for carbon dioxide (CO2) mitigation technologies as increasing emissions continue to threaten our environment. Carbon capture and storage (CCS) alone… (more)

▼ There is a pressing need for carbon dioxide (CO2) mitigation technologies as increasing emissions continue to threaten our environment. Carbon capture and storage (CCS) alone would not be able to achieve temperature rise below 2 °C. In addition, CCS cost increases considerably for power generation and other industries where CO2 separation is necessary. Conversion of CO2 to usable products is the most economical and feasible solution as it could offset CO2 separation cost. Liquid fuels are an attractive route since it is a commodity used globally and demand increases with population and economic growth. Conversion of CO 2 to liquid fuels would also reduce dependence on fossil fuels, increasing fuel economy security. This way CO2 would be recycled from emissions and transformed into fuel and then recycled again, potentially generating zero CO2 emissions, creating a closed carbon cycle. CO2 can be converted to liquid fuels using various technologies. For instance, biomass, algae, and photochemical technologies can be used to directly convert CO2 to fuels, while, photochemical and thermochemical can be used to convert CO2 to CO, which can subsequently be converted to liquid fuels. The latter has been regarded as the most efficient route currently and potentially in the future. Currently, thermochemical routes outperform photochemical in conversion rates and material recyclability over several cycles. Thermochemical CO2 conversion technologies include reverse water gas shift (RWGS), thermochemical cycles, and reverse water gas shift-chemical looping (RWGSCL). The differences between these technologies will be discussed in Section 1.2. RWGS-CL is a promising technology since it has achieved higher conversion rates than thermochemical cycles at lower operating temperatures. This is a two-step cyclic process, that first reduces a perovskite oxide (ABO 3) with hydrogen (H2) and subsequently oxidizes the oxygen vacant perovskite (ABO3-δ), thereby converting CO2 to CO and regenerating its structure. CO can subsequently be converted to hydrocarbons via Fischer Tropsch Synthesis. Performance of different perovskites compared to the state-of-the art material ceria (CeO2) are discussed in Section 1.3. Energy requirements are reduced by doping the A-site and B-site with alkaline earth and transition metals. Perovskites containing cobalt (Co), iron (Fe), and manganese (Mn) have exhibited either enhanced CO2 conversion, lower operating temperatures or higher stability. The specific studies showcasing these properties are discussed in Section 1.4. We aim to introduce these notable properties to achieve a high performing material by simultaneous doping of Co, Fe, and Mn into the B-site of a lanthanum perovskite. Three compositions, LaCo0.50Fe0.25Mn0.25O 3 (Co50), LaCo0.25Fe0.50Mn0.25O 3 (Fe50), and LaCo0.25Fe0.25Mn0.50O 3 (Mn50), were synthesized experimentally (Section 2.1) and modeled computationally (Section 2.5). Characterization techniques such as Xray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photo-electron…

Subjects/Keywords: carbon dioxide conversion; DFT; oxygen vacancy; reverse water gas shift-chemical looping; Chemical Engineering

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APA (6^th Edition):

Ramos, A. E. (2018). Enhanced CO₂ Conversion by the Simultaneous Doping of Co, Fe, and Mn in the B-site of a Lanthanum Perovskite. (Thesis). University of South Florida. Retrieved from https://scholarcommons.usf.edu/etd/8138

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Ramos, Adela E. “Enhanced CO₂ Conversion by the Simultaneous Doping of Co, Fe, and Mn in the B-site of a Lanthanum Perovskite.” 2018. Thesis, University of South Florida. Accessed April 17, 2021. https://scholarcommons.usf.edu/etd/8138.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Ramos, Adela E. “Enhanced CO₂ Conversion by the Simultaneous Doping of Co, Fe, and Mn in the B-site of a Lanthanum Perovskite.” 2018. Web. 17 Apr 2021.

Vancouver:

Ramos AE. Enhanced CO₂ Conversion by the Simultaneous Doping of Co, Fe, and Mn in the B-site of a Lanthanum Perovskite. [Internet] [Thesis]. University of South Florida; 2018. [cited 2021 Apr 17]. Available from: https://scholarcommons.usf.edu/etd/8138.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Ramos AE. Enhanced CO₂ Conversion by the Simultaneous Doping of Co, Fe, and Mn in the B-site of a Lanthanum Perovskite. [Thesis]. University of South Florida; 2018. Available from: https://scholarcommons.usf.edu/etd/8138

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Arizona

19. Zhang, Shuyang. Desulfurized Jet A Fuel Processing To Produce Hydrogen via Autothermal Reforming and Water-Gas Shift .

Degree: 2018, University of Arizona

URL: http://hdl.handle.net/10150/630165

► Hydrogen is an alternative fuel which is well recognized as one of the solutions to the fossil fuel depletion problem. As an energy carrier, hydrogen… (more)

▼ Hydrogen is an alternative fuel which is well recognized as one of the solutions to the fossil fuel depletion problem. As an energy carrier, hydrogen can be used to store and deliver energy or be converted into other types of energy, such as heat, electrical energy or mechanical work. Among all the applications, fuel cell is drawing increasing attention for its advantages such as higher theoretical energy conversion efficiency, no internal moving mechanical parts and environmentally friendly. Almost all the common fuel cells require hydrogen gas as the fuel source oxidized to complete the half-reaction redox cycle, which makes hydrogen gas a crucial factor for the development of fuel cell technique. However, under some certain circumstances, hydrogen supply could be extremely constrained by the harsh environment. For example, fuel cells used onboard has critical requirement on the space and extremely limited energy source, which makes carrying extra hydrogen tanks not an option in most cases. Therefore, onboard hydrogen production via catalytic autothermal reforming (ATR) and water-gas shift (WGS) is considered beneficial to vehicles using fuel cells as auxiliary power unit because it eliminates the challenges of hydrogen storage and delivery. The objective of this research is to develop a fuel processing system with reliable ATR and WGS catalysts to produce hydrogen feasibly from Jet A fuel, which is used as the primary fuel for both civilian and military transportation. Jet A fuel is expected to be converted into hydrogen gas, so that when considering onboard fuel cell applications, extra tanks of natural gas, ammonia or other hydrocarbons are not necessary. However, before the process can be examined, the sulfur component containing in the Jet A fuel must be removed because sulfur can easily poison the catalysts participating in the conversion reactions and even the catalysts in the downstream fuel cells. An effective and reliable in-house-made adsorbent was developed through simple procedures and cheap raw materials. The adsorbent has a very large surface area of over 250 m2/g with the optimal sulfur adsorption capacity of 2.95 mg-S/g-ads at the breakthrough point of 50 ppmw S in effluent fuel. A kwth-class fuel processing testing system was designed and fabricated afterwards in the lab to examine the system performance through experiments. The ATR of n-dodecane, working as the surrogate of Jet A fuel, was firstly studied with the initial simplified system under different operating conditions for better understanding each of the reactions. The compositions of system effluents in dry gas basis were detected by an on-site GC instrument and the gas temperature at distinct locations were monitored by a bunch of thermocouples connecting to a data acquisition (DAQ) system purchased from National Instruments company. Three indices, hydrogen yield, fuel conversion and energy efficiency were calculated based on the experimental results to evaluate the system performance. In addition, a novel in-house-made honeycomb-type… Advisors/Committee Members: Li, Peiwen (advisor), Chan, Cho Lik (committeemember), Zohar, Yitshak (committeemember), Farrell, James (committeemember).

Subjects/Keywords: autothermal reforming; fuel processing; heat exchanger; hydrogen production; self-sustainability; water-gas shift

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APA (6^th Edition):

Zhang, S. (2018). Desulfurized Jet A Fuel Processing To Produce Hydrogen via Autothermal Reforming and Water-Gas Shift . (Doctoral Dissertation). University of Arizona. Retrieved from http://hdl.handle.net/10150/630165

Chicago Manual of Style (16^th Edition):

Zhang, Shuyang. “Desulfurized Jet A Fuel Processing To Produce Hydrogen via Autothermal Reforming and Water-Gas Shift .” 2018. Doctoral Dissertation, University of Arizona. Accessed April 17, 2021. http://hdl.handle.net/10150/630165.

MLA Handbook (7^th Edition):

Zhang, Shuyang. “Desulfurized Jet A Fuel Processing To Produce Hydrogen via Autothermal Reforming and Water-Gas Shift .” 2018. Web. 17 Apr 2021.

Vancouver:

Zhang S. Desulfurized Jet A Fuel Processing To Produce Hydrogen via Autothermal Reforming and Water-Gas Shift . [Internet] [Doctoral dissertation]. University of Arizona; 2018. [cited 2021 Apr 17]. Available from: http://hdl.handle.net/10150/630165.

Council of Science Editors:

Zhang S. Desulfurized Jet A Fuel Processing To Produce Hydrogen via Autothermal Reforming and Water-Gas Shift . [Doctoral Dissertation]. University of Arizona; 2018. Available from: http://hdl.handle.net/10150/630165

20. Zhou, Mingxia. First-principles based micro-kinetic modeling for catalysts design.

Degree: PhD, Department of Chemical Engineering, 2018, Kansas State University

URL: http://hdl.handle.net/2097/38608

► Efficient and selective catalysis lies at the heart of many chemical reactions, enabling the synthesis of chemicals and fuels with enormous societal and technological impact.… (more)

▼ Efficient and selective catalysis lies at the heart of many chemical reactions, enabling the synthesis of chemicals and fuels with enormous societal and technological impact. A fundamental understanding of intrinsic catalyst properties for effective manipulation of the reactivity and selectivity of industrial catalysts is essential to select proper catalysts to catalyze the reactions we want and hinder the reactions we do not want. The progress in density functional theory (DFT) makes it possible to describe interfacial catalytic reactions and predict catalytic activities from one catalyst to another. In this study, water-gas shift reaction (WGSR) was used as a model reaction. First-principles based micro-kinetic modeling has been performed to deeply understand interactions between competing reaction mechanisms, and the relationship with various factors such as catalyst materials, structures, promoters, and interactions between intermediates (e.g., CO self-interaction) that govern the observed catalytic behaviors. Overall, in this thesis, all relevant reaction mechanisms in the model reaction on well-defined active sites were developed with first-principles calculations. With the established mechanism, the promotional effect of K adatom on Ni(111) on WGSR compared to the competing methanation was understood. Moreover, the WGSR kinetic trend, with the hydrogen production rate decreasing with increasing Ni particle diameters (due to the decreasing fractions of low-coordinated surface Ni site), was reproduced conveniently from micro-kinetic modeling techniques. Empirical correlations such as Brønsted-Evans-Polanyi (BEP) relationship for O-H, and C-O bond formation or cleavage on Ni(111), Ni(100), and Ni(211) were incorporated to accelerate computational analysis and generate trends on other transition metals (e.g., Cu, Au, Pt). To improve the numerical quality of micro-kinetic modeling, later interactions of main surface reaction intermediates were proven to be critical and incorporated successfully into the kinetic models. Finally, evidence of support playing a role in the enhancement of catalyst activity and the impact on future modeling will be discussed. DFT will be a powerful tool for understanding and even predicting catalyst performance and is shaping our approach to catalysis research. Such molecular-level information obtained from computational methods will undoubtedly guide the design of new catalyst materials with high precision. Advisors/Committee Members: Bin Liu.

Subjects/Keywords: Computational catalyst design; Density functional theory; Water-gas shift reaction; Transition metal catalysts

10 more images…

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APA (6^th Edition):

Zhou, M. (2018). First-principles based micro-kinetic modeling for catalysts design. (Doctoral Dissertation). Kansas State University. Retrieved from http://hdl.handle.net/2097/38608

Chicago Manual of Style (16^th Edition):

Zhou, Mingxia. “First-principles based micro-kinetic modeling for catalysts design.” 2018. Doctoral Dissertation, Kansas State University. Accessed April 17, 2021. http://hdl.handle.net/2097/38608.

MLA Handbook (7^th Edition):

Zhou, Mingxia. “First-principles based micro-kinetic modeling for catalysts design.” 2018. Web. 17 Apr 2021.

Vancouver:

Zhou M. First-principles based micro-kinetic modeling for catalysts design. [Internet] [Doctoral dissertation]. Kansas State University; 2018. [cited 2021 Apr 17]. Available from: http://hdl.handle.net/2097/38608.

Council of Science Editors:

Zhou M. First-principles based micro-kinetic modeling for catalysts design. [Doctoral Dissertation]. Kansas State University; 2018. Available from: http://hdl.handle.net/2097/38608

Lehigh University

21. Zhu, Minghui. Rational Design of High Temperature Water-Gas Shift Catalysts with Non-Toxic Earth-Abundant Elements.

Degree: PhD, Chemical Engineering, 2017, Lehigh University

URL: https://preserve.lehigh.edu/etd/2914

► The copper promoted chromium-iron oxide has for decades been used as the commercial catalyst for production of H2 via the High Temperature-Water Gas Shift reaction… (more)

▼ The copper promoted chromium-iron oxide has for decades been used as the commercial catalyst for production of H2 via the High Temperature-Water Gas Shift reaction (HT-WGS). The wide operation temperature range, high activity and robust thermostability has made this catalyst the catalyst of choice for HT-WGS. The toxic nature of hexavalent chromium has motivated extensive research to develop non-chromium HT-WGS catalysts. The lack of fundamental understanding of this HT-WGS catalyst system (catalyst structure under working conditions, reaction mechanism and copper/chromium promotion mechanism), however, have hampered the developed of Cr-free catalysts. The objectives of the dissertation were (1) to resolve the fundamentals of copper and chromium promotion mechanisms for the HT-WGS reaction, and (2) then apply the new fundamental insights to guide the rational design of chromium-free iron oxide-based HT-WGS catalysts. Temperature programmed surface reaction (TPSR) was employed to resolve the decades long debate regarding the HT-WGS reaction mechanism on iron oxide-based catalysts. Isotope C16O2/C18O2 switch experiments provided insights on the nature of active sites and the participation of surface oxygen, which allowed for the first time to calculate the Turnover Frequency (TOF) of iron oxide-based HT-WGS catalysts. To understand the structure of copper promoted chromium-iron oxide catalyst under reaction condition, a series of modern characterization techniques were employed (XRD, in situ Raman spectroscopy, Near Ambient Pressure X-ray Photoelectron Spectroscopy (NAP-XPS), High-Sensitivity Low-Energy Ion Scattering (HS-LEIS) Spectroscopy, in situ X-ray Absorption Spectroscopy and TEM-EDX). The activated catalysts were chemically probed with CO-Temperature Programmed Reduction (TPR) to examine the effects of copper and chromium on the catalyst activity for removing oxygen by CO, which is the rate-determining-step. These findings provided critical insights into the promotion mechanisms of copper and chromium. Finally, based on the fundamental understanding of the existing commercial catalysis system, new chromium-free, environmentally friendly iron oxide based HT-WGS catalysts were rationally designed. Advisors/Committee Members: Wachs, Israel E..

Subjects/Keywords: Catalysis; High Temperature; Hydrogen; Iron Based; Redox Mechanism; Water-Gas Shift; Chemical Engineering; Engineering

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APA (6^th Edition):

Zhu, M. (2017). Rational Design of High Temperature Water-Gas Shift Catalysts with Non-Toxic Earth-Abundant Elements. (Doctoral Dissertation). Lehigh University. Retrieved from https://preserve.lehigh.edu/etd/2914

Chicago Manual of Style (16^th Edition):

Zhu, Minghui. “Rational Design of High Temperature Water-Gas Shift Catalysts with Non-Toxic Earth-Abundant Elements.” 2017. Doctoral Dissertation, Lehigh University. Accessed April 17, 2021. https://preserve.lehigh.edu/etd/2914.

MLA Handbook (7^th Edition):

Zhu, Minghui. “Rational Design of High Temperature Water-Gas Shift Catalysts with Non-Toxic Earth-Abundant Elements.” 2017. Web. 17 Apr 2021.

Vancouver:

Zhu M. Rational Design of High Temperature Water-Gas Shift Catalysts with Non-Toxic Earth-Abundant Elements. [Internet] [Doctoral dissertation]. Lehigh University; 2017. [cited 2021 Apr 17]. Available from: https://preserve.lehigh.edu/etd/2914.

Council of Science Editors:

Zhu M. Rational Design of High Temperature Water-Gas Shift Catalysts with Non-Toxic Earth-Abundant Elements. [Doctoral Dissertation]. Lehigh University; 2017. Available from: https://preserve.lehigh.edu/etd/2914

University of Maryland

22. Gibbons, William Tilden. ELECTROSPUN CERIA-BASED FIBERS FOR ENERGY CONVERSION APPLICATIONS.

Degree: Chemical Engineering, 2014, University of Maryland

URL: http://hdl.handle.net/1903/15190

► Electrospun ceria-based fibers are explored for two energy conversion applications. An electrospinning facility was developed and the electrospinning process and subsequent fibrous material processing was… (more)

▼ Electrospun ceria-based fibers are explored for two energy conversion applications. An electrospinning facility was developed and the electrospinning process and subsequent fibrous material processing was optimized to enable rapid, scalable, and inexpensive production of ceramic fibers with diameters ranging from 50 nm to 5 μm. In this work, electrospinning of ceria-based fibers with various dopants were produced by spinning a sol with polyvinylypyrolidone (PVP), polar solvents, Ce(NO3)36H2O, and additional metal salts as desired. PVP removal by oxidation, followed by calcination in air, produced CeO2-based fibers. Non-woven ceramic textile mats were electrospun for integration into a compact water-gas-shift membrane reactor with a metallic Pd-based membrane for pure H2 production. The fibrous mats (CeO2 doped with 2 wt% Pd and/or 10 wt% Cu), were characterized for water-gas-shift (WGS) catalysis. High initial activity was followed by slow deactivation over 60 hours during time-on-stream testing at 400°C. Ex-situ characterization of the catalyst indicated that reduction and surface segregation of the Cu caused the deactivation which could be reversed by a brief oxidation treatment above 400°C. To test the Pd/Cu-doped ceria mats in the membrane reactor application, a H2-selective membrane system was constructed from a 5 μm-thick Pd/Cu (60/40 wt%) alloy foil supported on porous stainless steel. The electrospun fibers, mechanically pressed against the membrane foil, provided stable pure H2 production for over 300 hours at 400°C. The integration of the catalyst and H2 membrane achieved super-equilibrium conversion to H2 for some feed conditions. Though the membrane system showed stable performance, the oxidative treatments induced rapid membrane degradation, and are not a viable route for catalyst re-activation in such systems. A second application was investigated for the electrospun ceria-based fibers involving their use as a structured working material for solar-driven thermochemical redox cycles. These cycles use concentrated sunlight to drive endothermic oxide (CeO2) reduction at high temperatures (up to 1700 K) and lower temperature re-oxidation with CO2 and/or H2O to produce CO and/or H2 for subsequent fuel production. The electrospun fibers offer a cost-effective, flexible, and scalable path to the production of such working materials because the nature of the synthesis offers extensive composition control and the fiber structure reduces surface area loss at high temperatures. Un-doped CeO2 as well as Zr and Pr doped CeO2 fibers were studied to understand the affect of high temperature exposure on the overall structure of powder and fiber materials, and the affect of dopant concentration and structure on reduction and fuel production kinetics. Under the conditions studied, Pr doping (5/10 mol %) promoted grain growth, and did not improve reduction yields over un-doped CeO2. Doping with Zr (2.5, 5, 10, 20 mol %) inhibited sintering, increased reduction yields, and slowed oxidation kinetics.… Advisors/Committee Members: Jackson, Gregory S (advisor).

Subjects/Keywords: Energy; Chemical engineering; Catalyst; Ceria; Electrospinning; Energy Conversion Materials; Solar Thermal; Water Gas Shift

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APA (6^th Edition):

Gibbons, W. T. (2014). ELECTROSPUN CERIA-BASED FIBERS FOR ENERGY CONVERSION APPLICATIONS. (Thesis). University of Maryland. Retrieved from http://hdl.handle.net/1903/15190

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Gibbons, William Tilden. “ELECTROSPUN CERIA-BASED FIBERS FOR ENERGY CONVERSION APPLICATIONS.” 2014. Thesis, University of Maryland. Accessed April 17, 2021. http://hdl.handle.net/1903/15190.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Gibbons, William Tilden. “ELECTROSPUN CERIA-BASED FIBERS FOR ENERGY CONVERSION APPLICATIONS.” 2014. Web. 17 Apr 2021.

Vancouver:

Gibbons WT. ELECTROSPUN CERIA-BASED FIBERS FOR ENERGY CONVERSION APPLICATIONS. [Internet] [Thesis]. University of Maryland; 2014. [cited 2021 Apr 17]. Available from: http://hdl.handle.net/1903/15190.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Gibbons WT. ELECTROSPUN CERIA-BASED FIBERS FOR ENERGY CONVERSION APPLICATIONS. [Thesis]. University of Maryland; 2014. Available from: http://hdl.handle.net/1903/15190

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Cincinnati

23. Arvanitis, Antonios. High Temperature High Pressure Water Gas Shift Reaction in Zeolite Membrane Reactors.

Degree: PhD, Engineering and Applied Science: Chemical Engineering, 2019, University of Cincinnati

URL: http://rave.ohiolink.edu/etdc/view?acc_num=ucin1563872266361549

► The water gas shift (WGS) reaction of syngas (mainly containing CO, CO2, and H2) and subsequent H2/CO2 separation are key operations for H2 production from… (more)

▼ The water gas shift (WGS) reaction of syngas (mainly containing CO, CO2, and H2) and subsequent H2/CO2 separation are key operations for H2 production from fossil fuels, agricultural and forestry biomass, and municipal wastes with pre-combustion CO2 capture in thermal electric power production by the emerging integrated gasification-combined cycle (IGCC) power plants. Hydrogen permselective membrane reactors (MR) are capable of achieving near complete CO conversion (?CO) with simultaneous H2/CO2 separation that can substantially simplify and intensify the process to lower the overall operation cost. However, up to date, there is a lack of WGS MRs, which are practically viable either due to membrane instability in the WGS reaction of real syngas or insufficient ?CO and H2 recovery (RH2). This dissertation reports the development and scale up of thermally and chemically stable tubular zeolite membranes for future industrial high temperature and high pressure WGS MR to achieve nearly complete ?CO when nearly total RH2 is achieved in the permeate stream.An effective in-situ crystallization method has been established for synthesizing MFI-type zeolite membranes on industrially meaningful low-cost commercial porous a-alumina tube supports. The zeolite membranes with a length of 35 cm exhibited a H2/CO2 selectivity (aH2/CO2) ranging from 10 to 45 and hydrogen permeance (Pm,H2), of 1 – 2*10-7 mol/m2·Pa·s at 500 °C. The WGS reaction in the single tube zeolite MR has been studied at high temperature (500 °C) and high pressure (20bar) using nanocrystalline Fe-based catalysts under practically meaningful space velocities and steam-to-CO ratios. The zeolite membranes with moderate aH2/CO2 and Pm,H2, exceeded the equilibrium conversion at >500 °C and achieved ?CO >99.9%. Realization of near-complete ?CO must rely on the prevention of excessive permeation of CO when the membrane has imperfect H2/CO selectivity. For the porous membranes with imperfect H2/CO permeation selectivity, such as the zeolite membranes in this research, the arrangement of catalyst loading along the membrane tube length has shown significant influences on the ?CO. For near-complete ?CO, the CO must be largely converted through the pre-membrane section so that CO partial pressure becomes sufficiently low to prevent excessive CO leak to the permeate side. A simple one-dimensional isothermal PFR model has been established for simulation of the WGS reaction in the zeolite membrane tubes with large lengths and small diameters. Both the experimental investigations and model calculations have indicated that such a distributed catalyst packing is effective for obtaining total removal of H2 and negligible escape of unreacted CO to accomplish near-complete ?CO (>99.5%). Such packing significantly improves the performance of the MR compared to the uniform packing of catalyst with the same load.Finally, because of the limited aH2/CO2, the H2 purity in the permeate stream is moderate when achieving total removal of H2 from the reaction side. A highly CO2-selective polymeric… Advisors/Committee Members: Dong, Junhang (Committee Chair).

Subjects/Keywords: Chemical Engineering; Water-Gas-Shift; Zeolites; Membrane Reactor; High Pressure; High Temperature

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Arvanitis, A. (2019). High Temperature High Pressure Water Gas Shift Reaction in Zeolite Membrane Reactors. (Doctoral Dissertation). University of Cincinnati. Retrieved from http://rave.ohiolink.edu/etdc/view?acc_num=ucin1563872266361549

Chicago Manual of Style (16^th Edition):

Arvanitis, Antonios. “High Temperature High Pressure Water Gas Shift Reaction in Zeolite Membrane Reactors.” 2019. Doctoral Dissertation, University of Cincinnati. Accessed April 17, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1563872266361549.

MLA Handbook (7^th Edition):

Arvanitis, Antonios. “High Temperature High Pressure Water Gas Shift Reaction in Zeolite Membrane Reactors.” 2019. Web. 17 Apr 2021.

Vancouver:

Arvanitis A. High Temperature High Pressure Water Gas Shift Reaction in Zeolite Membrane Reactors. [Internet] [Doctoral dissertation]. University of Cincinnati; 2019. [cited 2021 Apr 17]. Available from: http://rave.ohiolink.edu/etdc/view?acc_num=ucin1563872266361549.

Council of Science Editors:

Arvanitis A. High Temperature High Pressure Water Gas Shift Reaction in Zeolite Membrane Reactors. [Doctoral Dissertation]. University of Cincinnati; 2019. Available from: http://rave.ohiolink.edu/etdc/view?acc_num=ucin1563872266361549

University of Cincinnati

24. Yun, Seonguk. Sulfur Tolerant Supported Bimetallic Catalysts for Low Temperature Water Gas Shift Reaction.

Degree: PhD, Engineering and Applied Science: Chemical Engineering, 2019, University of Cincinnati

URL: http://rave.ohiolink.edu/etdc/view?acc_num=ucin1573224656177825

► A series of model CuPd nanoparticles, CoMo oxide nanoparticles, different metal oxide supported Mo sulfide catalysts, and sets of different composition ratio and surface coverage… (more)

▼ A series of model CuPd nanoparticles, CoMo oxide nanoparticles, different metal oxide supported Mo sulfide catalysts, and sets of different composition ratio and surface coverage of CoMo sulfide catalysts were prepared and investigated as sulfur-tolerant WGS catalysts. For comparison, monometallic catalysts prepared by incipient wetness impregnation, as well as commercial CoMo catalysts, were also investigated. The model CoMo-S catalysts at the monolayer surface coverage employed in this research are highly promising as sulfur-tolerant WGS catalysts displaying desirable structural, morphological, and compositional properties.The CuPd-2 catalysts maximized the number of WGS-active Cu⁰ sites with the optimized ratio (2.37) of CuO/CuAl₂O₄, showing higher WGS activity, thermal stability, and sulfur tolerance at 250°C than any other tested Cu-based catalysts. Cu-Pd bimetallic alloy catalysts showed enhanced reducibility due to the Pd-promoting effect through hydrogen spillover and additional reducible CuO sites through Cu species diffusion from the CuO shell to Al₂O₃. The Mo and CoMo oxide nanoparticles were prepared by a metal colloid chemical co-reduction method by modifying the concentrations of the Mo and Co precursors during synthesis. The WGS activity of n-Mo-S and n-CoMo-S catalysts increased due to the reduction of the average particle size up to 5-Mo and 10-CoMo. The extent of sulfidation of n-Mo-S catalysts was saturated at 5-Mo and correlated with WGS activity. 10-CoMo-S catalysts were the most active among the tested Al2O3-supported Mo-based catalysts with similar sulfur dependence to a commercial CoMo/MgO catalyst. Mo-S/ZrO₂ showed the highest WGS activity in 1,000 ppm H₂S-containing feed and lowest H₂S dependence in H₂S-free feed among ZrO_2-, Al₂O_3-, TiO2-, CeO_2-, and SiO₂-supported Mo catalysts. Weak support-MoO₃ interaction of ZrO₂ favored a higher extent of sulfidation, correlated to the WGS activity, and stable sulfur bonding in Mo-S/ZrO₂ led to low sulfur dependence. Mo_5-S/ZrO₂ at monolayer MoO₃ coverage showed optimal WGS activity and extent of sulfidation, suggesting that the topmost Mo-S layer comprised WGS-active catalytic sites. CoMo-S/ZrO₂ catalyst at monolayer CoMo-O coverage with Co/Mo = 0.3 catalysts was the most active WGS catalyst among all the tested catalysts in this study. This catalyst was thermally stable for at least 4 weeks of reaction test, and demonstrated low sulfur tolerance under H2S-free feed at 350°C and GHSV 35,000 h^-1. Structurally, this catalyst exhibited optimized surface coverage, highly dispersed CoMo-S species, saturated extent of sulfidation, and optimal number of active sites.The important result of this study is that cobalt promoter facilitated the dispersion of CoMo-S species, the formation of active surface sulfur, and the… Advisors/Committee Members: Guliants, Vadim (Committee Chair).

Subjects/Keywords: Chemical Engineering; Water gas shift reaction; Mo sulfide; surface coverage; nanoparticle; heterogeneous catalysis

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Yun, S. (2019). Sulfur Tolerant Supported Bimetallic Catalysts for Low Temperature Water Gas Shift Reaction. (Doctoral Dissertation). University of Cincinnati. Retrieved from http://rave.ohiolink.edu/etdc/view?acc_num=ucin1573224656177825

Chicago Manual of Style (16^th Edition):

Yun, Seonguk. “Sulfur Tolerant Supported Bimetallic Catalysts for Low Temperature Water Gas Shift Reaction.” 2019. Doctoral Dissertation, University of Cincinnati. Accessed April 17, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1573224656177825.

MLA Handbook (7^th Edition):

Yun, Seonguk. “Sulfur Tolerant Supported Bimetallic Catalysts for Low Temperature Water Gas Shift Reaction.” 2019. Web. 17 Apr 2021.

Vancouver:

Yun S. Sulfur Tolerant Supported Bimetallic Catalysts for Low Temperature Water Gas Shift Reaction. [Internet] [Doctoral dissertation]. University of Cincinnati; 2019. [cited 2021 Apr 17]. Available from: http://rave.ohiolink.edu/etdc/view?acc_num=ucin1573224656177825.

Council of Science Editors:

Yun S. Sulfur Tolerant Supported Bimetallic Catalysts for Low Temperature Water Gas Shift Reaction. [Doctoral Dissertation]. University of Cincinnati; 2019. Available from: http://rave.ohiolink.edu/etdc/view?acc_num=ucin1573224656177825

University of Cincinnati

25. Chakraborty, Arundhoti. Development of Copper Catalysts for the Reduction of Polar Bonds.

Degree: PhD, Arts and Sciences: Chemistry, 2016, University of Cincinnati

URL: http://rave.ohiolink.edu/etdc/view?acc_num=ucin1479814963555246

► This thesis focuses on the synthesis of new transition metal complexes that show metal–metal cooperativity and metal-ligand cooperativity. Late-late and early-late heterobimetallic complexes have been… (more)

▼ This thesis focuses on the synthesis of new transition metal complexes that show metal–metal cooperativity and metal-ligand cooperativity. Late-late and early-late heterobimetallic complexes have been synthesized and employed in important chemical transformations like benzaldehyde (PhCHO) reduction under water-gas shift reaction (WGSR) conditions and reduction of an imine moiety respectively. A bifunctional hexameric copper hydride complex has also been isolated and utilized in the catalytic hydrogenation of aldehydes, ketones and CO2.I have synthesized late-late heterobimetallic complexes containing Fe–Cu bonds where the iron center is supported by a Knolker-type cyclopentadienone ligand and the copper center is ligated to a N-heterocyclic carbene. Reactions between the Knolker’s iron tricarbonyl complexes (SiMe3 and tBu derivatives) and (IPr)CuOH lead to the formation of new Fe/Cu heterobimetallic complexes that contain a bridging hydride in the solid state. Solution IR, ¹³C{¹H} NMR analysis and variable temperature NMR suggest a dominant terminal iron hydride structure in solution for the SiMe3 derivative.Stoichiometric reactions of these Fe/Cu complexes with alkyl halides lead to the formation of new Fe/Cu halide complexes. Under a CO atmosphere, these Fe/Cu complexes generate the corresponding iron tricarbonyl species and the dimeric (IPr)CuH complex. Reduction of PhCHO to PhCH2OH was successfully performed under water-gas shift reaction conditions. Both metal centers are necessary to carry out the reaction demonstrating the importance of metal-metal cooperativity. Isotope labelling studies performed with ¹³CO confirmed that the Fe/Cu catalyst is indeed active in WGSR. In my second project I have synthesized and isolated a new copper hydride supported by a bis(phosphine)amine [iPrPN(H)P] ligand with a hexameric copper core. The assignment of the hydride peak in the ¹H NMR spectrum was confirmed by comparing the ¹H NMR spectrum of the related copper deuteride complex. Benzaldehyde and acetophenone insert into the Cu-H bond to afford the corresponding copper alkoxide products. CO2 also undergoes a facile insertion into the Cu-H bond to form the corresponding copper formate species. Isotope labelling study indicates that the insertion is reversible but favors the formation of copper formate. Hydrogenation of aldehydes, ketones and CO2 has been carried out with the copper bromide precursor under mild conditions. The copper hydride complex also serves as an effective catalyst in the hydrogenation of benzaldehyde implying its direct involvement in the catalytic reaction. Catalytic inactivity of the copper bromide species containing the [iPr(PN(Me)P] ligand in the hydrogenation reaction implies a bifunctional mechanism; however, further investigation is needed to support this mechanism.My third project focuses on the synthesis of early-late heterobimetallic complexes containing Cr–Cu bonds and the respective metal centers are supported by bulky Cp* (Cp* = 1,2,3,4,5-cyclopentadienyl) and… Advisors/Committee Members: Guan, Hairong (Committee Chair).

Subjects/Keywords: Chemistry; Organometallic Chemistry; cooperativity; heterobimetallic complexes; iron and copper catalysis; Water-Gas Shift Reaction; hydrogenation

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APA (6^th Edition):

Chakraborty, A. (2016). Development of Copper Catalysts for the Reduction of Polar Bonds. (Doctoral Dissertation). University of Cincinnati. Retrieved from http://rave.ohiolink.edu/etdc/view?acc_num=ucin1479814963555246

Chicago Manual of Style (16^th Edition):

Chakraborty, Arundhoti. “Development of Copper Catalysts for the Reduction of Polar Bonds.” 2016. Doctoral Dissertation, University of Cincinnati. Accessed April 17, 2021. http://rave.ohiolink.edu/etdc/view?acc_num=ucin1479814963555246.

MLA Handbook (7^th Edition):

Chakraborty, Arundhoti. “Development of Copper Catalysts for the Reduction of Polar Bonds.” 2016. Web. 17 Apr 2021.

Vancouver:

Chakraborty A. Development of Copper Catalysts for the Reduction of Polar Bonds. [Internet] [Doctoral dissertation]. University of Cincinnati; 2016. [cited 2021 Apr 17]. Available from: http://rave.ohiolink.edu/etdc/view?acc_num=ucin1479814963555246.

Council of Science Editors:

Chakraborty A. Development of Copper Catalysts for the Reduction of Polar Bonds. [Doctoral Dissertation]. University of Cincinnati; 2016. Available from: http://rave.ohiolink.edu/etdc/view?acc_num=ucin1479814963555246

New Jersey Institute of Technology

26. Zhu, Yuan. CO2 reduction over noble metal/carbon nanotube catalyst.

Degree: PhD, Chemical, Biological and Pharmaceutical Engineering, 2017, New Jersey Institute of Technology

URL: https://digitalcommons.njit.edu/dissertations/50

► Carbon nanotube-based Pt/Pd and Ru catalysts, independently synthesized by a microwave reaction technique, show good catalytic activity for CO2 reduction in the contexts of… (more)

Subjects/Keywords: Dry reforming; Reverse water gas shift; Carbon Nanotube; Kinetics modeling; Chemical Engineering

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Zhu, Y. (2017). CO2 reduction over noble metal/carbon nanotube catalyst. (Doctoral Dissertation). New Jersey Institute of Technology. Retrieved from https://digitalcommons.njit.edu/dissertations/50

Chicago Manual of Style (16^th Edition):

Zhu, Yuan. “CO2 reduction over noble metal/carbon nanotube catalyst.” 2017. Doctoral Dissertation, New Jersey Institute of Technology. Accessed April 17, 2021. https://digitalcommons.njit.edu/dissertations/50.

MLA Handbook (7^th Edition):

Zhu, Yuan. “CO2 reduction over noble metal/carbon nanotube catalyst.” 2017. Web. 17 Apr 2021.

Vancouver:

Zhu Y. CO2 reduction over noble metal/carbon nanotube catalyst. [Internet] [Doctoral dissertation]. New Jersey Institute of Technology; 2017. [cited 2021 Apr 17]. Available from: https://digitalcommons.njit.edu/dissertations/50.

Council of Science Editors:

Zhu Y. CO2 reduction over noble metal/carbon nanotube catalyst. [Doctoral Dissertation]. New Jersey Institute of Technology; 2017. Available from: https://digitalcommons.njit.edu/dissertations/50

27. MACIEL, Leonardo José Lins. Processos Catalíticos Associados de Conversão do Gás Natural Em Hidrogênio e Coprodutos.

Degree: 2012, Universidade Federal de Pernambuco

URL: https://repositorio.ufpe.br/handle/123456789/11880

►

CAPES, CTPetro e CNPq

Produção de hidrogênio de elevadas purezas e coprodutos têm sido objeto de desenvolvimentos de tecnologias usando o gás natural como matéria-prima… (more)

▼

CAPES, CTPetro e CNPq

Produção de hidrogênio de elevadas purezas e coprodutos têm sido objeto de desenvolvimentos de tecnologias usando o gás natural como matéria-prima com processamento catalítico como a desidroaromatização (DAM) associada à reforma seca (RSM) em um leito duplo com ocorrência de coprodutos em condições não oxidativas. As produções de hidrogênio previstas objetivam a utilização do monóxido de carbono de efluentes de reformas do gás natural, via reação water gas shift (WGS) e o desenvolvimento de catalisadores avançados de metais preciosos em fases dispersas sobre um suporte. Como objetivo desta pesquisa pode-se citar: i) Desenvolvimento de uma tecnologia usando o gás natural como matéria-prima para produção de hidrogênio de alta pureza, e coprodutos tais como gás de síntese e acetileno como intermediários para formulação de aromáticos, principalmente o benzeno, via desidroaromatização e a reforma seca, em condições não oxidativas, com utilização de reator de leito fixo. ii) Desenvolvimento de novos catalisadores de Pt e Au (formulação e caracterização) e o estudo detalhado dos parâmetros cinéticos, mecanisticos e em diversos suportes e seus efeitos para reação de WGS. Operações de processamento do metano em reator de leito fixo nas condições: 525°C, 550°C, 575°C, 1 atm, 155-180 cm3/min, fração molar Ar :CH4, 0,5:0,5 de metano e argônio para DAM e relação molar Ar :CH4:CO2, 0,57:0,27:0,16 para DAM/RSM. As operações em reator de leito fixo na presença da mistura dos catalisadores (2,60%)Mo-(0,5%)Ru/HZSM e (11,23%)Ni/ -Al2O3, como resultado principal apresentaram uma acentuada produção de acetileno (42,91%) e moderadas produções de hidrogênio e monóxido de carbono (16%-56% H2 e 1,45% CO, 575°C). No processo catalítico de WGS foram estudados catalisadores de platina e ouro em baixas temperaturas (120°C – 300°C) para manter a conversão total de CO nas condições diferenciais abaixo de 10%. O fluxo total de entrada foi mantido constante com uma composição padrão de gás de 6,8% CO, 8,5% CO2, 21,9% H2O e 37,4% H2. A temperatura foi variada numa faixa entre 20° e 30°C, para determinação da energia de ativação aparente. Aplicações de metodologia da cinética de processos catalíticos permitiram estimar valores de baixas energias de ativação (catalisador Pt: 53 kJ/mol – 63 kJ/mol; catalisador Au:11 kJ/mol –95 kJ/mol), os quais confirmaram os bons níveis de atividade dos catalisadores formulados para o processo WGS, com destaque para os catalisadores 2%Pt/TiO2, 2%Au/ZrO2 e 2%Au/TiO2.

Advisors/Committee Members: ABREU, Cesar Augusto Moraes de, BENACHOUR, Mohand, RIBEIRO, Fabio H..

Subjects/Keywords: Desidroaromatização; Reforma Seca do Metano; Water Gas Shift; Acetileno; Hidrogênio; Reator de Leito Fixo Diferencial

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

MACIEL, L. J. L. (2012). Processos Catalíticos Associados de Conversão do Gás Natural Em Hidrogênio e Coprodutos. (Doctoral Dissertation). Universidade Federal de Pernambuco. Retrieved from https://repositorio.ufpe.br/handle/123456789/11880

Chicago Manual of Style (16^th Edition):

MACIEL, Leonardo José Lins. “Processos Catalíticos Associados de Conversão do Gás Natural Em Hidrogênio e Coprodutos.” 2012. Doctoral Dissertation, Universidade Federal de Pernambuco. Accessed April 17, 2021. https://repositorio.ufpe.br/handle/123456789/11880.

MLA Handbook (7^th Edition):

MACIEL, Leonardo José Lins. “Processos Catalíticos Associados de Conversão do Gás Natural Em Hidrogênio e Coprodutos.” 2012. Web. 17 Apr 2021.

Vancouver:

MACIEL LJL. Processos Catalíticos Associados de Conversão do Gás Natural Em Hidrogênio e Coprodutos. [Internet] [Doctoral dissertation]. Universidade Federal de Pernambuco; 2012. [cited 2021 Apr 17]. Available from: https://repositorio.ufpe.br/handle/123456789/11880.

Council of Science Editors:

MACIEL LJL. Processos Catalíticos Associados de Conversão do Gás Natural Em Hidrogênio e Coprodutos. [Doctoral Dissertation]. Universidade Federal de Pernambuco; 2012. Available from: https://repositorio.ufpe.br/handle/123456789/11880

University of California – Riverside

28. Thanmongkhon, Yoothana. The Production of High Levels of Renewable Natural Gas from Biomass Using Steam Hydrogasification.

Degree: Chemical and Environmental Engineering, 2014, University of California – Riverside

URL: http://www.escholarship.org/uc/item/6qh949sb

► Renewable Natural Gas (RNG) has been identified as an important alternative fuel that can help to achieve a number of national goals related to the… (more)

Subjects/Keywords: Chemical engineering; Biomass and Biosolids; Methane and Hydrogen; Process Demonstration Unit; Renewable Natural Gas; Steam Hydrogasification; Water Gas Shift

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APA (6^th Edition):

Thanmongkhon, Y. (2014). The Production of High Levels of Renewable Natural Gas from Biomass Using Steam Hydrogasification. (Thesis). University of California – Riverside. Retrieved from http://www.escholarship.org/uc/item/6qh949sb

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Thanmongkhon, Yoothana. “The Production of High Levels of Renewable Natural Gas from Biomass Using Steam Hydrogasification.” 2014. Thesis, University of California – Riverside. Accessed April 17, 2021. http://www.escholarship.org/uc/item/6qh949sb.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Thanmongkhon, Yoothana. “The Production of High Levels of Renewable Natural Gas from Biomass Using Steam Hydrogasification.” 2014. Web. 17 Apr 2021.

Vancouver:

Thanmongkhon Y. The Production of High Levels of Renewable Natural Gas from Biomass Using Steam Hydrogasification. [Internet] [Thesis]. University of California – Riverside; 2014. [cited 2021 Apr 17]. Available from: http://www.escholarship.org/uc/item/6qh949sb.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Thanmongkhon Y. The Production of High Levels of Renewable Natural Gas from Biomass Using Steam Hydrogasification. [Thesis]. University of California – Riverside; 2014. Available from: http://www.escholarship.org/uc/item/6qh949sb

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

University of Michigan

29. Schaidle, Joshua A. Carbide and Nitride Based Catalysts for Synthesis Gas Conversion.

Degree: PhD, Chemical Engineering, 2011, University of Michigan

URL: http://hdl.handle.net/2027.42/89768

► The production of fuels and chemicals from syngas (H2 and CO) plays a critical role in our economy and will play an even greater role… (more)

▼ The production of fuels and chemicals from syngas (H2 and CO) plays a critical role in our economy and will play an even greater role in the future as we transition from petroleum-derived products to biomass-derived products. This transition will require new catalysts that exhibit high activities, selectivities and durabilities for syngas conversion reactions. Research described in this dissertation investigated the catalytic properties of early transition metal carbide and nitride based materials for two industrially relevant syngas conversion reactions: water gas shift (WGS) and Fischer-Tropsch Synthesis (FTS). In addition to kinetic measurements, the materials were characterized using bulk and surface techniques to develop structure-function relationships. For WGS, the effects of sulfur on the catalytic performance and structures of Mo2C and Pt/Mo2C catalysts were investigated. In the presence of 5 ppm H2S, Mo2C deactivated by 90% from its initial activity and was only partially regenerable. The deactivation was caused by the formation of MoS2 on the catalyst surface. These domains are known to be slightly active for WGS. Oxygen deposited on the Mo2C surface under reaction conditions may have facilitated the formation of MoS2, suggesting that minimizing the amount of surface oxygen could lead to improved sulfur tolerance. Pt/Mo2C was irreversibly poisoned by H2S, primarily due to the formation of PtS. For FTS, the rates were a function of the metal and the interstitial atom, suggesting that it may be possible to tune the activity of the catalyst. The intrinsic rate trend for the carbide and nitride materials was as follows: Mo2C ~ W2C ~ VN ~ NbN > Mo2N, W2N >> VC, NbC. The materials were capable of direct CO dissociation, a key step in the production of hydrocarbons. Mo2N appeared to catalyze the FTS reaction via the carbide mechanism while Mo2C catalyzed either the oxygenate or CO-insertion mechanism. Regarding selectivity, the materials favored light hydrocarbons and CO2. The latter may have been a consequence of the high WGS activities for these catalysts. Based on these results, the early transition metal carbides and nitrides may be promising catalysts for the production of short chain hydrocarbons or olefins from biomass-derived syngas. Advisors/Committee Members: Thompson Jr, Levi T. (committee member), Gulari, Erdogan (committee member), Sanford, Melanie (committee member), Schwank, Johannes W. (committee member).

Subjects/Keywords: Fischer-Tropsch; Catalyst; Water Gas Shift; Early Transition Metal Carbide; X-ray Absorption Spectroscopy; Synthesis Gas; Chemical Engineering; Engineering

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Schaidle, J. A. (2011). Carbide and Nitride Based Catalysts for Synthesis Gas Conversion. (Doctoral Dissertation). University of Michigan. Retrieved from http://hdl.handle.net/2027.42/89768

Chicago Manual of Style (16^th Edition):

Schaidle, Joshua A. “Carbide and Nitride Based Catalysts for Synthesis Gas Conversion.” 2011. Doctoral Dissertation, University of Michigan. Accessed April 17, 2021. http://hdl.handle.net/2027.42/89768.

MLA Handbook (7^th Edition):

Schaidle, Joshua A. “Carbide and Nitride Based Catalysts for Synthesis Gas Conversion.” 2011. Web. 17 Apr 2021.

Vancouver:

Schaidle JA. Carbide and Nitride Based Catalysts for Synthesis Gas Conversion. [Internet] [Doctoral dissertation]. University of Michigan; 2011. [cited 2021 Apr 17]. Available from: http://hdl.handle.net/2027.42/89768.

Council of Science Editors:

Schaidle JA. Carbide and Nitride Based Catalysts for Synthesis Gas Conversion. [Doctoral Dissertation]. University of Michigan; 2011. Available from: http://hdl.handle.net/2027.42/89768

University of California – Irvine

30. Rosner, Fabian. Techno-Economic Analysis of IGCCs Employing Novel Warm Gas Carbon Dioxide Separation and Carbon Capture Enhancements for High-Methane Syngas.

Degree: Mechanical and Aerospace Engineering, 2018, University of California – Irvine

URL: http://www.escholarship.org/uc/item/2cp6p4bd

► The utilization of coal worldwide for electric power generation portends a need for advanced technologies to mitigate the release of carbon. To this end, a… (more)

Subjects/Keywords: Engineering; Energy; Sustainability; Carbon Capture; Integrated Gasification Combined Cycle (IGCC); Isothermal Shifting; Transport Gasifier (TRIG); Warm Gas Cleanup; Water Gas Shift

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APA · Chicago · MLA · Vancouver · CSE | Export to Zotero / EndNote / Reference Manager

APA (6^th Edition):

Rosner, F. (2018). Techno-Economic Analysis of IGCCs Employing Novel Warm Gas Carbon Dioxide Separation and Carbon Capture Enhancements for High-Methane Syngas. (Thesis). University of California – Irvine. Retrieved from http://www.escholarship.org/uc/item/2cp6p4bd

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Chicago Manual of Style (16^th Edition):

Rosner, Fabian. “Techno-Economic Analysis of IGCCs Employing Novel Warm Gas Carbon Dioxide Separation and Carbon Capture Enhancements for High-Methane Syngas.” 2018. Thesis, University of California – Irvine. Accessed April 17, 2021. http://www.escholarship.org/uc/item/2cp6p4bd.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

MLA Handbook (7^th Edition):

Rosner, Fabian. “Techno-Economic Analysis of IGCCs Employing Novel Warm Gas Carbon Dioxide Separation and Carbon Capture Enhancements for High-Methane Syngas.” 2018. Web. 17 Apr 2021.

Vancouver:

Rosner F. Techno-Economic Analysis of IGCCs Employing Novel Warm Gas Carbon Dioxide Separation and Carbon Capture Enhancements for High-Methane Syngas. [Internet] [Thesis]. University of California – Irvine; 2018. [cited 2021 Apr 17]. Available from: http://www.escholarship.org/uc/item/2cp6p4bd.

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

Council of Science Editors:

Rosner F. Techno-Economic Analysis of IGCCs Employing Novel Warm Gas Carbon Dioxide Separation and Carbon Capture Enhancements for High-Methane Syngas. [Thesis]. University of California – Irvine; 2018. Available from: http://www.escholarship.org/uc/item/2cp6p4bd

Note: this citation may be lacking information needed for this citation format:
Not specified: Masters Thesis or Doctoral Dissertation

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Open Access Theses and Dissertations