subject:(Bioinorganic Chemistry)

1. Dixon, Natalie Anne. Bio-Inspired Modulation of Tris(triazolyl)borate’s Electronic Properties Resulting in Enhanced Reactivity of Cu(I/II) and Other Transition Metal Complexes.

Degree: 2013, Drexel University

URL: http://hdl.handle.net/1860/4365

► The natural design of enzymes and proteins inspires synthetic strategies for designing more efficient transition metal catalysts for achieving similar organic transformations. Novel tris(triazolyl)borate ligands… (more)

Subjects/Keywords: Chemistry; Bioinorganic chemistry; Ligands

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APA (6^th Edition):

Dixon, N. A. (2013). Bio-Inspired Modulation of Tris(triazolyl)borate’s Electronic Properties Resulting in Enhanced Reactivity of Cu(I/II) and Other Transition Metal Complexes. (Thesis). Drexel University. Retrieved from http://hdl.handle.net/1860/4365

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):

Dixon, Natalie Anne. “Bio-Inspired Modulation of Tris(triazolyl)borate’s Electronic Properties Resulting in Enhanced Reactivity of Cu(I/II) and Other Transition Metal Complexes.” 2013. Thesis, Drexel University. Accessed January 15, 2021. http://hdl.handle.net/1860/4365.

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

MLA Handbook (7^th Edition):

Dixon, Natalie Anne. “Bio-Inspired Modulation of Tris(triazolyl)borate’s Electronic Properties Resulting in Enhanced Reactivity of Cu(I/II) and Other Transition Metal Complexes.” 2013. Web. 15 Jan 2021.

Vancouver:

Dixon NA. Bio-Inspired Modulation of Tris(triazolyl)borate’s Electronic Properties Resulting in Enhanced Reactivity of Cu(I/II) and Other Transition Metal Complexes. [Internet] [Thesis]. Drexel University; 2013. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/1860/4365.

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

Council of Science Editors:

Dixon NA. Bio-Inspired Modulation of Tris(triazolyl)borate’s Electronic Properties Resulting in Enhanced Reactivity of Cu(I/II) and Other Transition Metal Complexes. [Thesis]. Drexel University; 2013. Available from: http://hdl.handle.net/1860/4365

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

Texas A&M University

2. Liu, Tianbiao. Organometallic Complexes that Model the Active Sites of the [FeFe]- and [Fe]-Hydrogenases.

Degree: PhD, Chemistry, 2011, Texas A&M University

URL: http://hdl.handle.net/1969.1/ETD-TAMU-2009-12-7344

► My research primarily focuses on biomimetics of the active sites of the [FeFe]- and [Fe]-hydrogenases (H2ase) and is classified into three parts. Part A: The… (more)

▼ My research primarily focuses on biomimetics of the active sites of the [FeFe]- and [Fe]-hydrogenases (H2ase) and is classified into three parts. Part A: The one-electron oxidation of asymmetrically disubstituted FeIFeI models of the active site of the [FeFe]-H2ase, (mu-pdt)[Fe(CO)2PMe3][Fe(CO)2NHC] (pdt = 1,3- propanedithiolate, NHC = N-heterocyclic carbene) generates mixed valent FeIIFeI models of the Hox state of [FeFe]-hydrogenase. The spectroscopic properties, structures, reactivities and relative stabilities of the one-electron oxidized mixed valent complexes, (mu-pdt)(mu-CO)[FeII(CO)2PMe3][FeI(CO)NHC]+ are discussed in the context of experimental and theoretical data and biological relevance. Part B: DFT computations find the Fe-Fe bond in the FeIFeI diiron models ((mu- pdt)[Fe(CO)2L][Fe(CO)2L'] ( L, L' = CO, PPh3, or PMe3) is thermodynamically favored to produce the mu-oxo or oxidative addition product, FeII-O-FeII, nevertheless the sulfurbased HOMO-1 accounts for the experimentally observed mono- and bis-O-atom adducts at sulfur. The FeII(mu-H)FeII diiron model, (mu-pdt)(mu-H)[Fe(CO)2PMe3]2 (IV-5), for which the HOMO is largely of sulfur character, exclusively yields S-oxygenation. Deoxygenation with reclamation of the mu-pdt parent complexes occurs in a proton/electron coupled process. The possible biological relevance of oxygenation and deoxygenation studies is discussed. Comprehensive investigations of intramolecular CO site change and intermolecular CO/L (L = PMe3 or CN-) exchange of (mu-pst)[Fe(CO)3]2 (IV-1-O), (mu-pdt)[Fe(CO)3]2 (V-1), and their mono-CN-/PMe3 substituted derivatives indicated that the factors influencing the rate of the CO/L exchange reaction of such diiron carbonyls are intramolecular structural rearrangement (or fluxionality) and nucleophilic attack by the incoming ligand. Part C: X-ray diffraction and spectroscopic studies of a series of mono- and disubstituted complexes, FeI2(CO)xL4-x, x = 2 or 3, showed them to be rudimentary structural models of the [Fe]-H2ase active site in native (FeII(CO)2) or CO-inhibited (FeII(CO)3) states. Full characterization of the advanced model complexes ((NS)FeI(CO)2P, NS = 2-amidophenothiolate; P = phosphine) including x-ray diffraction, DFT computations, and Mossbauer studies revealed the interesting "noninnocent" character of these complexes due to the NS ligand. Ligand-based protonation with a strong acid, HBF4Et2O, interrupted the pi-delocalization over Fe and ligand of complex VII-1 and switched on CO uptake (1 bar) and 12CO/ 13CO exchange of VII-1. The intermediate, VII-1-H+, capable of CO uptake, was defined by DFT calculations. Advisors/Committee Members: Darensbourg, Marcetta Y. (advisor), Hall, Michael B. (committee member), Soriaga, Manuel P. (committee member), Barondeau, David P. (committee member), Balbuena, Perla B. (committee member).

Subjects/Keywords: Diiron dithiolate; bioinorganic chemistry; hydrogenase.

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APA (6^th Edition):

Liu, T. (2011). Organometallic Complexes that Model the Active Sites of the [FeFe]- and [Fe]-Hydrogenases. (Doctoral Dissertation). Texas A&M University. Retrieved from http://hdl.handle.net/1969.1/ETD-TAMU-2009-12-7344

Chicago Manual of Style (16^th Edition):

Liu, Tianbiao. “Organometallic Complexes that Model the Active Sites of the [FeFe]- and [Fe]-Hydrogenases.” 2011. Doctoral Dissertation, Texas A&M University. Accessed January 15, 2021. http://hdl.handle.net/1969.1/ETD-TAMU-2009-12-7344.

MLA Handbook (7^th Edition):

Liu, Tianbiao. “Organometallic Complexes that Model the Active Sites of the [FeFe]- and [Fe]-Hydrogenases.” 2011. Web. 15 Jan 2021.

Vancouver:

Liu T. Organometallic Complexes that Model the Active Sites of the [FeFe]- and [Fe]-Hydrogenases. [Internet] [Doctoral dissertation]. Texas A&M University; 2011. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/1969.1/ETD-TAMU-2009-12-7344.

Council of Science Editors:

Liu T. Organometallic Complexes that Model the Active Sites of the [FeFe]- and [Fe]-Hydrogenases. [Doctoral Dissertation]. Texas A&M University; 2011. Available from: http://hdl.handle.net/1969.1/ETD-TAMU-2009-12-7344

University of Johannesburg

3. Koekemoer, Leigh-Anne. Assessing toxicity of FeMn dust particles collected from a South African ferromanganese smelter works : in vitro studies on primary rat astrocytes and BEAS-2B cells.

Degree: 2014, University of Johannesburg

URL: http://hdl.handle.net/10210/11360

►

M.Sc. (Biochemistry)

Manganese (Mn) is an essential trace element. Although it is vital for the normal development of mammals, too much Mn can be harmful.… (more)

▼

M.Sc. (Biochemistry)

Manganese (Mn) is an essential trace element. Although it is vital for the normal development of mammals, too much Mn can be harmful. Most reported cases of toxicity have been found in occupational settings, such as welding, mining and ferro-manganese (FeMn) production plants. Long-term overexposure to Mn can result in lung epithelial necrosis and the development of a neurological disease, manganism. Even though evidence of Mn-associated diseases exists, some epidemiological studies have found no association between occupational exposure levels and possible indicators of neurotoxic effects. It is, therefore, important to establish Mn toxicity and the mechanisms involved in this toxicity, for a possible identification of biomarkers of exposure and effect. The hypothesis formulated states that, FeMn particulate matter consists of nano and micro sized particles that, upon inhalation, may cause injury to the lungs and translocate to the brain. Since Mn-induced injury to the brain and lungs is a possibility, this study aimed to investigate the effects of FeMn dust, which was collected from a FeMn smelter works, on primary rat astrocytes and human bronchial epithelial (BEAS-2B) cells. This was achieved by first characterizing the physicochemical properties of the particles by using a scanning mobility particle sizer (SMPS) and aerodynamic particle sizer (APS) for size distribution, Brunauer-Emmett-Teller (BET) for surface area determination and inductively coupled plasma atomic emission spectroscopy (ICP-AES) for elemental composition analysis. Cells were treated with 5, 10, 25 μg/cm2 FeMn, and particle uptake, by astrocytes and BEAS-2B cells, was confirmed using dark field microscopy e.g. Cytoviva® hyperspectral imaging system. The viability and toxicity of FeMn was studied using the conventional toxicity assay systems, including 3-bis [2-Methoxy-4- nitro-5-sulfophenyl]-2H-tetrazolium-5-carboxyanilide salt (XTT), adenosine triphosphate (ATP) and lactate dehydrogenase (LDH) assays. It was, however, established that FeMn particles interfere with the final read-out produced by some of these assay systems. Therefore, a rare application of the xCELLigence real time cell analysis (RTCA) system was implemented, as a better option, in the assessment of the toxicity and viability of cells in the presence of FeMn particles. The ability of FeMn particles to cause deoxyribonucleic acid (DNA) damage in both cell types was also determined using the alkaline comet assay. Finally, the nuclear translocation of the antioxidant transcription factor nuclear factor erythroid 2-related factor 2 (Nrf2) and inflammatory transcription factor nuclear factor kappa B (Nf-κB), was studied using Western blotting. The results showed that FeMn, in a dose dependent manner, could enter the cell, decrease the viability, induce DNA damage, and initiate nuclear transport of the studied transcription factors. The same methodologies were implemented to determine the physicochemical properties of Min- U-Sil 5 crystalline silica, used as…

Subjects/Keywords: Ferromanganese - Toxicology; Bioinorganic chemistry

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

APA (6^th Edition):

Koekemoer, L. (2014). Assessing toxicity of FeMn dust particles collected from a South African ferromanganese smelter works : in vitro studies on primary rat astrocytes and BEAS-2B cells. (Thesis). University of Johannesburg. Retrieved from http://hdl.handle.net/10210/11360

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):

Koekemoer, Leigh-Anne. “Assessing toxicity of FeMn dust particles collected from a South African ferromanganese smelter works : in vitro studies on primary rat astrocytes and BEAS-2B cells.” 2014. Thesis, University of Johannesburg. Accessed January 15, 2021. http://hdl.handle.net/10210/11360.

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

MLA Handbook (7^th Edition):

Koekemoer, Leigh-Anne. “Assessing toxicity of FeMn dust particles collected from a South African ferromanganese smelter works : in vitro studies on primary rat astrocytes and BEAS-2B cells.” 2014. Web. 15 Jan 2021.

Vancouver:

Koekemoer L. Assessing toxicity of FeMn dust particles collected from a South African ferromanganese smelter works : in vitro studies on primary rat astrocytes and BEAS-2B cells. [Internet] [Thesis]. University of Johannesburg; 2014. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/10210/11360.

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

Council of Science Editors:

Koekemoer L. Assessing toxicity of FeMn dust particles collected from a South African ferromanganese smelter works : in vitro studies on primary rat astrocytes and BEAS-2B cells. [Thesis]. University of Johannesburg; 2014. Available from: http://hdl.handle.net/10210/11360

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

4. Neupane, Kosh P. Nickel Superoxide Dismutase: Insight Into The Metalloenzyme Gained From Functional Metallopeptide Models.

Degree: 2009, University of Nevada – Reno

URL: http://hdl.handle.net/11714/4114

► Superoxide (O2*-) is one of the toxic reactive oxygen species produced in the mitochondrial respiratory chain during ATP synthesis. All organisms have evolved defense systems… (more)

▼ Superoxide (O2*-) is one of the toxic reactive oxygen species produced in the mitochondrial respiratory chain during ATP synthesis. All organisms have evolved defense systems capable of destroing O2*- before it can cause cellular damage. The most widely utilized O2*- detoxification pathway involves metalloenzymes called superoxide dismutases. Based on the metal cofactors present in the active site of the enzymes they are classified into Cu/ZnSOD, MnSOD, FeSOD or NiSOD. Nickel superoxide dismutase (NiSOD) is the most recently discovered SOD, and is found in Streptomyces species and cyanobacteria. The active site of NiSOD utilizes a unique coordination environment. In its reduced state, NiII is coordinated by the N-terminal amine from His1, the amide nitrogen from Cys2, and two cis-thiolates from Cys2 and Cys6 affording a square planar coordination geometry about nickel. Upon oxidation to NiIII, the imidazole of His1 becomes the fifth ligand to nickel affording a square pyramidal geometry about nickel. To understand the contributions of this unique coordination environment utilized by NiSOD we have chosen a metallopeptide based mimicking approach. We have synthesized and characterized a series of synthetic metallopeptide maquettes of NiSOD based on the first 12 amino acid residues from the N-terminus end of S. coelicolor NiSOD. These have been used to investigate the influence of amine/amide vs. bis-amide coordination in NiSOD. Results show that [NiII(SODM1-Ac)] is a poorer SOD than [NiII(SODM1)]. This seems to indicate why nature has chosen the mixture of amine and amide nitrogen ligands at the NiSOD active-site: bis-amide ligation (as is found at the NiN2S2 center of acetyl-coenzyme-A synthase) would produce a poor SOD. We have also probed the role of the axial ligand His(1) on the catalytic activity of NiSOD. We find that His(1) tunes the redox potential towards the mid point potential of the superoxide oxidation and reduction process, and hence accelerates catalysis. Based on our inhibition studies of [NiII(SODM2)] by cyanide and the O2*- mimic azide, superoxide dimutation by NiSOD appears to be taking place by an outer-sphere mechanism. We also probed the influence of some of the non-coordinating amino acid residues in NiSOD to delineate their possible role. Although some amino acids residues such as His(1), Cys(2), Pro(5) and Cys(6) in the Ni-binding hook of NiSOD are conserved, some bacterial species possess variation of the non-coordinating amino acids found in the Ni-binding hook of S. coelicolor NiSOD. Also investigated is the influence of H-bonding of e-imidazole nitrogen of His1. The result shows that H-bonding makes the NiIII-dN weaker, and enhances the catalysis. Advisors/Committee Members: Shearer, Jason M. (advisor), Catalano, Vincent J. (committee member), Frost, Brian J. (committee member), Phaneuf, Ronald A. (committee member), Pardini, Ronald S. (committee member).

Subjects/Keywords: Bioinorganic Chemistry

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APA (6^th Edition):

Neupane, K. P. (2009). Nickel Superoxide Dismutase: Insight Into The Metalloenzyme Gained From Functional Metallopeptide Models. (Thesis). University of Nevada – Reno. Retrieved from http://hdl.handle.net/11714/4114

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):

Neupane, Kosh P. “Nickel Superoxide Dismutase: Insight Into The Metalloenzyme Gained From Functional Metallopeptide Models.” 2009. Thesis, University of Nevada – Reno. Accessed January 15, 2021. http://hdl.handle.net/11714/4114.

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

MLA Handbook (7^th Edition):

Neupane, Kosh P. “Nickel Superoxide Dismutase: Insight Into The Metalloenzyme Gained From Functional Metallopeptide Models.” 2009. Web. 15 Jan 2021.

Vancouver:

Neupane KP. Nickel Superoxide Dismutase: Insight Into The Metalloenzyme Gained From Functional Metallopeptide Models. [Internet] [Thesis]. University of Nevada – Reno; 2009. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/11714/4114.

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

Council of Science Editors:

Neupane KP. Nickel Superoxide Dismutase: Insight Into The Metalloenzyme Gained From Functional Metallopeptide Models. [Thesis]. University of Nevada – Reno; 2009. Available from: http://hdl.handle.net/11714/4114

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

University of California – Irvine

5. Paretsky, Jonathan Daniel. Streptavidin as a Host for Copper(II) Complexes.

Degree: Chemistry, 2015, University of California – Irvine

URL: http://www.escholarship.org/uc/item/3834f5zt

► In nature, metal ions are utilized in many proteins and enzymes in order to perform a variety of chemical transformations that are essential to maintaining… (more)

▼ In nature, metal ions are utilized in many proteins and enzymes in order to perform a variety of chemical transformations that are essential to maintaining human life. The range of selectivity and functionality can be attributed to the unique environment surrounding each active site, which allow for control over not only the primary coordination sphere—containing atoms covalently bound to the metal ion, but also the secondary coordination sphere (microenvironment)—made up of non-covalent interactions such as hydrogen bonds (H-bonds). Although nature is very efficient at these chemical processes, achieving the same level of selectivity is difficult in synthetic systems. In order to reproduce the functions found in metalloproteins it is necessary to maintain control over both the primary and secondary coordination spheres of synthetic systems as seen within active sites. To accomplish this, typically a rigid organic framework is constructed that will coordinate to a metal ion and additionally provide a supporting network of non-covalent interactions: intramolecular H-bonds. The Borovik group has performed extensive research the area of secondary coordination sphere effects around transition metal complexes and has developed a multitude of ligand frameworks that bind metal ions and incorporate intramolecular H-bond donors or acceptors that can stabilize exogenous ligands bound to the transition metal (TM) complexes. While these systems have been extremely effective and have been used to prepare unique high-valent metal-oxo/hydroxo species, they fall short in being able to provide extensive networks of H-bonds and long-range interactions found in microenvironments of metalloproteins. To address these challenges and gain further control over the secondary coordination sphere, this dissertation presents the development of new research program within the Borovik group in collaboration with the Ward lab: the development of artificial metalloproteins using biotin-Streptavidin (Sav) technology. Although Sav does not naturally contain metal ions, TM complexes of interest can be attached to biotin and inserted into the protein. This is an attractive feature, because of Sav’s exceptionally high affinity for biotin , which can be exploited for the use of installing biotinylated metal complexes. Furthermore, the selective binding of biotin provides a reproducible anchor for TM complexes within the active site of protein. In addition to being able to chemically modify a ligand, the protein is amenable to site directed mutagenesis, which allows for alterations of the microenvironment around the TM complexes. This combined chemogenetic approach allows for enhanced control over primary and secondary coordination spheres of TM complexes. The first portion of this document describes the study of biotinylated copper(II) complexes with varied linker lengths between the Cu(II) complex and biotin. Utilizing different linker lengths was proposed to allow for: 1) to design discrete monomeric species confined within separate…

Subjects/Keywords: Chemistry; Artificial Metalloenzymes; Bioinorganic Chemistry; Metalliobiochemistry; Streptavidin

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

APA (6^th Edition):

Paretsky, J. D. (2015). Streptavidin as a Host for Copper(II) Complexes. (Thesis). University of California – Irvine. Retrieved from http://www.escholarship.org/uc/item/3834f5zt

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):

Paretsky, Jonathan Daniel. “Streptavidin as a Host for Copper(II) Complexes.” 2015. Thesis, University of California – Irvine. Accessed January 15, 2021. http://www.escholarship.org/uc/item/3834f5zt.

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

MLA Handbook (7^th Edition):

Paretsky, Jonathan Daniel. “Streptavidin as a Host for Copper(II) Complexes.” 2015. Web. 15 Jan 2021.

Vancouver:

Paretsky JD. Streptavidin as a Host for Copper(II) Complexes. [Internet] [Thesis]. University of California – Irvine; 2015. [cited 2021 Jan 15]. Available from: http://www.escholarship.org/uc/item/3834f5zt.

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

Council of Science Editors:

Paretsky JD. Streptavidin as a Host for Copper(II) Complexes. [Thesis]. University of California – Irvine; 2015. Available from: http://www.escholarship.org/uc/item/3834f5zt

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

Nelson Mandela Metropolitan University

6. Moleko-Boyce, Pulleng. Design of metal ion-selective reagents for recovery of precious metals.

Degree: 2019, Nelson Mandela Metropolitan University

URL: http://hdl.handle.net/10948/42510

► The study is divided into two sections; namely, (1) the design of rhodium(III) specific chelating ligands (tridentate bis-benzimidazole derivatives), and (2) the development of iridium(IV)-specific… (more)

▼ The study is divided into two sections; namely, (1) the design of rhodium(III) specific chelating ligands (tridentate bis-benzimidazole derivatives), and (2) the development of iridium(IV)-specific quaternary diammonium cations with electron donating and electron withdrawing groups. Bis-benzimidazole chelating ligands used were bis((1H-benzimidazol-2-yl)methyl)amine (NNN1), bis((1H-benzimidazol-2-yl)ethyl)amine (NNN2), bis((1H-benzimidazol-2-yl)methyl)sulfide (NSN1) and bis((1H-benzimidazol-2-yl)ethyl)sulfide (NSN2). Quaternary diammonium cations used were tetramethylbenzyl-1,10-diammonium chloride (QuatDMDAMeBnz), tetrabenzyl-1,10-diammonium chloride (QuatDMDABnz), tetratrifluoromethylbenzyl-1,10-diammonium chloride (QuatDMDACF3Bnz) and tetranitrobenzyl-1,10-diammonium chloride (QuatDMDANO2Bnz). For both studies, polyvinylbenzylchloride (PVBC) nanofibers were used as support material. The PVBC nanofibers which were functionalised with bis-benzimidazole derivatives and quaternary diammonium cations, respectively, were investigated for the selectivity for Rh(III) over Ir(III), Pt(II), Pd(II) and Ni(II), and for separation of Ir(IV) from Rh(III), respectively. The sorbent materials were characterised by FTIR, SEM, BET surface area, TGA, EDS and elemental analysis, and the results showed that the functionalization of the sorbent materials was successful.The efficiency of bis-benzimidazole derivatives and quaternary diammonium cations, respectively, were investigated in a column study under dynamic flow adsorption conditions. The adsorption kinetics and isotherms were investigated under batch conditions and fitted on pseudo-first-order and pseudo-second-order model, and Freundlich and Langmuir isotherm, respectively. It was observed that the bis-benzimidazole derivatives showed uptake of [RhCl3(H2O)3], and the loading capacities were observed in the following order; NSN1 (181.06 mg/g) > NSN2 (148.55 mg/g) > NNN1 (131.88 mg/g) > NNN2 (75.87 mg/g). The bis-benzimidazole derivatives preference for metal ions was further investigated with a multi-element solution containing Rh(III), Ir(III), Pt(II), Pd(II) and Ni(II). The bis-benzimidazole derivatives showed the following order of loading capacity: NSN1 (47.28 mg/g) > NSN2 (23.89 mg/g) > NNN1 (17.47 mg/g) > NNN2 (14.91 mg/g) for Rh(III); NSN2 (10.64 mg/g) > NNN2 (6.84 mg/g) > NSN1 (5.74 mg/g) > NNN1 (5.02 mg/g) for Ir(III); NNN2 (33.96 mg/g) > NSN1 (30.95 mg/g) > NSN2 (19.95 mg/g) > NNN1 (14.92 mg/g) for Pt(II); NNN1 (47.94 mg/g) > NNN2 (28.90 mg/g) > NSN1 (16.22 mg/g) > NSN2 (15.83 mg/g) for Pd(II). Bis-benzimidazole derivatives showed no uptake of nickel(II) under these conditions. It was observed the ligand-selectivity order for Rh(III) was similar in both single-element and multi-element studies. This order showed that the bis-benzimidazoles containing a sulfur atom showed a high preference for rhodium(III) compared to Pt(II) which had a high preference for NNN2 as well as Pd(II) which had a high preference for NNN1. Ir(III) generally had a lower preference for the…

Subjects/Keywords: Bioinorganic chemistry; Metal complexes; Speciation (Chemistry)

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

APA (6^th Edition):

Moleko-Boyce, P. (2019). Design of metal ion-selective reagents for recovery of precious metals. (Thesis). Nelson Mandela Metropolitan University. Retrieved from http://hdl.handle.net/10948/42510

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):

Moleko-Boyce, Pulleng. “Design of metal ion-selective reagents for recovery of precious metals.” 2019. Thesis, Nelson Mandela Metropolitan University. Accessed January 15, 2021. http://hdl.handle.net/10948/42510.

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

MLA Handbook (7^th Edition):

Moleko-Boyce, Pulleng. “Design of metal ion-selective reagents for recovery of precious metals.” 2019. Web. 15 Jan 2021.

Vancouver:

Moleko-Boyce P. Design of metal ion-selective reagents for recovery of precious metals. [Internet] [Thesis]. Nelson Mandela Metropolitan University; 2019. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/10948/42510.

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

Council of Science Editors:

Moleko-Boyce P. Design of metal ion-selective reagents for recovery of precious metals. [Thesis]. Nelson Mandela Metropolitan University; 2019. Available from: http://hdl.handle.net/10948/42510

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

University of Oregon

7. Osborn, Maire. Cellular RNA Targeting by Platinum (II) Anticancer Therapeutics.

Degree: PhD, Department of Chemistry and Biochemistry, 2014, University of Oregon

URL: http://hdl.handle.net/1794/17920

► Cis-diamminedichloroplatinum (II), or cisplatin, is a widely prescribed anticancer compound, currently one of only three platinum (II) complexes FDA approved for cancer treatment. Despite its… (more)

▼ Cis-diamminedichloroplatinum (II), or cisplatin, is a widely prescribed anticancer compound, currently one of only three platinum (II) complexes FDA approved for cancer treatment. Despite its widespread use, we lack a comprehensive picture of global drug targets, which would lend valuable insights into the molecular mechanisms of action and resistance in different tissues. Drug binding to genomic DNA is an accepted cause of downstream apoptotic signaling, but less than 10% of Pt (in the case of cisplatin) accumulates within genomic DNA. Non-genomic contributions to cisplatin's therapeutic action are also under active investigation. In particular, cisplatin treatment can disrupt RNA-based processes such as splicing and translation. Pt(II) targeting of non-DNA species such as RNA may contribute to or sensitize a cell to the downstream effects of this drug, including the induction of apoptosis. Chapter I summarizes the activity profile of Pt(II) therapeutics, describing cellular uptake, cellular localization, incidences of Pt(II) accumulation within RNA, and RNA processes affected following drug treatment. Chapter II reports our thorough investigation of the distribution of Pt species throughout messenger and ribosomal RNA, with the discovery that Saccharomyces cerevisiae ribosomes act as a de facto cellular Pt sponge. In Chapter III, we report the synthesis of an azide-functionalized platinum (II) species, picazoplatin, for post-treatment click labeling and isolation of drug targets in vivo. Picazoplatin was designed to circumvent mislocalization and misprocessing of Pt typically encountered when trying to track small molecules tethered to large, charged fluorophores. This chapter contains several proof-of-principle studies validating the use of this class of reagents for future purification and sequencing of Pt-bound nucleic acids. Chapter IV describes the first application of the click-capable Pt reagent technology: the demonstration of significant in-gel fluorescent detection of Pt-bound ribosomal RNA and transfer RNA extracted from picazoplatin-treated S. cerevisiae and the first evidence that cellular tRNA is a platinum substrate. Chapter V summarizes these data, which suggest a potential ribotoxic mechanism for cisplatin cytotoxicity and broadly describe a convenient click chemistry methodology that can be applied to identify other metal or covalent modification-based drug targets. This dissertation includes previously published and unpublished co-authored material. Advisors/Committee Members: Hawley, Diane (advisor).

Subjects/Keywords: Bioinorganic chemistry; Platinum anticancer therapeutics; RNA

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APA (6^th Edition):

Osborn, M. (2014). Cellular RNA Targeting by Platinum (II) Anticancer Therapeutics. (Doctoral Dissertation). University of Oregon. Retrieved from http://hdl.handle.net/1794/17920

Chicago Manual of Style (16^th Edition):

Osborn, Maire. “Cellular RNA Targeting by Platinum (II) Anticancer Therapeutics.” 2014. Doctoral Dissertation, University of Oregon. Accessed January 15, 2021. http://hdl.handle.net/1794/17920.

MLA Handbook (7^th Edition):

Osborn, Maire. “Cellular RNA Targeting by Platinum (II) Anticancer Therapeutics.” 2014. Web. 15 Jan 2021.

Vancouver:

Osborn M. Cellular RNA Targeting by Platinum (II) Anticancer Therapeutics. [Internet] [Doctoral dissertation]. University of Oregon; 2014. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/1794/17920.

Council of Science Editors:

Osborn M. Cellular RNA Targeting by Platinum (II) Anticancer Therapeutics. [Doctoral Dissertation]. University of Oregon; 2014. Available from: http://hdl.handle.net/1794/17920

Duke University

8. Franks, Andrew Thomas. Development of Stimulus-Responsive Ligands for the Modulation of Copper and Iron Coordination .

Degree: 2014, Duke University

URL: http://hdl.handle.net/10161/9034

► The ability to manipulate the coordination chemistry of metal ions has significant ramifications for the study and treatment of metal-related health concerns, including iron… (more)

▼ The ability to manipulate the coordination chemistry of metal ions has significant ramifications for the study and treatment of metal-related health concerns, including iron overload, UV skin damage, and microbial infection among many other conditions. To address this concern, chelating agents that change their metal binding characteristics in response to external stimuli have been synthesized and characterized by several spectroscopic and chromatographic analytical methods. The primary stimuli of interest for this work are light and hydrogen peroxide. Herein we report the previously unrecognized photochemistry of aroylhydrazone metal chelator ((E)-N′-[1-(2-hydroxyphenyl)ethyliden]isonicotinoylhydrazide) (HAPI) and its relation to HAPI metal binding properties. Based on promising initial results, a series of HAPI analogues was prepared to probe the structure-function relationships of aroylhydrazone photochemistry. These efforts elucidate the tunable nature of several aroylhydrazone photoswitching properties. Ongoing efforts in this laboratory seek to develop compounds called prochelators that exhibit a switch from low to high metal binding affinity upon activation by a stimulus of interest. In this context, we present new strategies to install multiple desired functions into a single structure. The prochelator 2-((E)-1-(2-isonicotinoylhydrazono)ethyl)phenyl (E)-3-(2,4-dihydroxyphenyl)acrylate (PC-HAPI) is masked with a photolabile trans-cinnamic acid protecting group that releases umbelliferone, a UV-absorbing, antioxidant coumarin along with a chelating agent upon UV irradiation. In addition to the antioxidant effects of the coumarin, the released chelator (HAPI) inhibits metal-catalyzed production of damaging reactive oxygen species. Finally a peroxide-sensitive prochelator quinolin-8-yl (Z)-3-(4-hydroxy-2-((4-(4,4,5,5-tetramethyl-1,3,2-dioxaborolan-2-yl)benzyl)oxy)phenyl)acrylate (BCQ) has been prepared using a novel synthetic route for functionalized cis-cinnamate esters. BCQ uses a novel masking strategy to trigger a 90-fold increase in fluorescence emission, along with the release of a desired chelator, in the presence of hydrogen peroxide. Advisors/Committee Members: Franz, Katherine J (advisor).

Subjects/Keywords: Chemistry; bioinorganic; chelator; coumarin; oxidative stress; photolabile

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APA (6^th Edition):

Franks, A. T. (2014). Development of Stimulus-Responsive Ligands for the Modulation of Copper and Iron Coordination . (Thesis). Duke University. Retrieved from http://hdl.handle.net/10161/9034

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):

Franks, Andrew Thomas. “Development of Stimulus-Responsive Ligands for the Modulation of Copper and Iron Coordination .” 2014. Thesis, Duke University. Accessed January 15, 2021. http://hdl.handle.net/10161/9034.

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

MLA Handbook (7^th Edition):

Franks, Andrew Thomas. “Development of Stimulus-Responsive Ligands for the Modulation of Copper and Iron Coordination .” 2014. Web. 15 Jan 2021.

Vancouver:

Franks AT. Development of Stimulus-Responsive Ligands for the Modulation of Copper and Iron Coordination . [Internet] [Thesis]. Duke University; 2014. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/10161/9034.

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

Council of Science Editors:

Franks AT. Development of Stimulus-Responsive Ligands for the Modulation of Copper and Iron Coordination . [Thesis]. Duke University; 2014. Available from: http://hdl.handle.net/10161/9034

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

University of Vermont

9. Conger, Matthew A. Spectroscopic Insight into Oxidative Heme Cleavage by the Non-canonical Heme Oxygenase IsdG from Staphylococcus aureus.

Degree: PhD, Chemistry, 2018, University of Vermont

URL: https://scholarworks.uvm.edu/graddis/944

► IsdG and IsdI are non-canonical heme oxygenases (HO) from Staphylococcus aureus that catalyze the oxidative cleavage of heme to give novel organic products (staphylobilins)… (more)

▼ IsdG and IsdI are non-canonical heme oxygenases (HO) from Staphylococcus aureus that catalyze the oxidative cleavage of heme to give novel organic products (staphylobilins) and iron as a nutrient for the pathogen. Comparison of the reported equilibrium dissociation constant (Kd) values for heme from IsdG and IsdI compared to the reported concentration of the labile heme pool called into question whether these enzymes are competent HOs in vivo. We took advantage of a second-sphere Trp whose fluorescence is quenched upon heme binding, which led to Kd values 2-3 orders of magnitude smaller than reported in the literature. Importantly, these Kd values were on the same order of magnitude as human HO, precluding design of a competitive inhibitor as an effective therapeutic. Based upon the kinetic and equilibrium data, and the finding that the half-life of IsdG is increased 2.5-fold by the presence of heme, we proposed IsdG is the main HO involved in iron acquisition which motivated further characterization of IsdG. IsdG-catalyzed heme catabolism proceeds through ferric-peroxoheme and meso-hydroxyheme intermediates en route to staphylobilin. A second-sphere Asn is known to be critical for enzymatic function, but its role in heme cleavage was unknown. Site-directed mutagenesis was employed to probe the role of Asn using ferric-azidoheme and ferric-cyanoheme as models of the putative ferric-peroxoheme intermediate. An optical spectroscopic study established that a hydrogen-bond between Asn and the iron-ligating (α) atom of the distal ligand perturbs the heme electronic structure. Density functional theory (DFT) suggested this hydrogen-bond triggers rotation of the distal ligand, which was corroborated by circular dichroism (CD), and delocalizes spin density onto the meso carbons. Electron paramagnetic resonance (EPR) revealed the Asn hydrogen-bond increases the Fe 3dxy character in the singly occupied molecular orbital (SOMO), a mechanism that can increase spin density on the meso carbons. Finally, the Asn hydrogen-bond moves the meso carbon resonances downfield in the 13C nuclear magnetic resonance (NMR) spectrum, consistent with excess spin density, confirming a DFT-predicted, Asn-induced spin delocalization. These results suggest IsdG funnels the reactivity of ferric-peroxoheme toward heme hydroxylation through an Asn-dependent bridged transition state, circumventing production of reactive, uncontrolled intermediates. Advisors/Committee Members: Matthew D. Liptak.

Subjects/Keywords: Bioinorganic Chemistry; Heme Oxygenase; Spectroscopy; Inorganic Chemistry; Physical Chemistry

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APA (6^th Edition):

Conger, M. A. (2018). Spectroscopic Insight into Oxidative Heme Cleavage by the Non-canonical Heme Oxygenase IsdG from Staphylococcus aureus. (Doctoral Dissertation). University of Vermont. Retrieved from https://scholarworks.uvm.edu/graddis/944

Chicago Manual of Style (16^th Edition):

Conger, Matthew A. “Spectroscopic Insight into Oxidative Heme Cleavage by the Non-canonical Heme Oxygenase IsdG from Staphylococcus aureus.” 2018. Doctoral Dissertation, University of Vermont. Accessed January 15, 2021. https://scholarworks.uvm.edu/graddis/944.

MLA Handbook (7^th Edition):

Conger, Matthew A. “Spectroscopic Insight into Oxidative Heme Cleavage by the Non-canonical Heme Oxygenase IsdG from Staphylococcus aureus.” 2018. Web. 15 Jan 2021.

Vancouver:

Conger MA. Spectroscopic Insight into Oxidative Heme Cleavage by the Non-canonical Heme Oxygenase IsdG from Staphylococcus aureus. [Internet] [Doctoral dissertation]. University of Vermont; 2018. [cited 2021 Jan 15]. Available from: https://scholarworks.uvm.edu/graddis/944.

Council of Science Editors:

Conger MA. Spectroscopic Insight into Oxidative Heme Cleavage by the Non-canonical Heme Oxygenase IsdG from Staphylococcus aureus. [Doctoral Dissertation]. University of Vermont; 2018. Available from: https://scholarworks.uvm.edu/graddis/944

10. Berto, Timothy C. Synthetic, Spectroscopic, and Theoretical Investigations into the Interactions and Detoxification of Nitric Oxide in Biology.

Degree: PhD, Chemistry, 2012, University of Michigan

URL: http://hdl.handle.net/2027.42/96117

► Bacterial nitric oxide reductase (NorBC) is responsible for NO reduction in denitrifying bacteria. This enzyme contains a dinuclear heme/non-heme iron active site in which the… (more)

Subjects/Keywords: Bioinorganic Chemistry; Chemistry; Science

…HCOs are able to perform NOR chemistry and NorBC is able to perform HCO chemistry, albeit at… …Lancaster, J. R., Jr., In Encyclopedia of Inorganic Chemistry, Bruce, R. B., Ed. Wiley: Chichester…

11 more images…

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APA (6^th Edition):

Berto, T. C. (2012). Synthetic, Spectroscopic, and Theoretical Investigations into the Interactions and Detoxification of Nitric Oxide in Biology. (Doctoral Dissertation). University of Michigan. Retrieved from http://hdl.handle.net/2027.42/96117

Chicago Manual of Style (16^th Edition):

Berto, Timothy C. “Synthetic, Spectroscopic, and Theoretical Investigations into the Interactions and Detoxification of Nitric Oxide in Biology.” 2012. Doctoral Dissertation, University of Michigan. Accessed January 15, 2021. http://hdl.handle.net/2027.42/96117.

MLA Handbook (7^th Edition):

Berto, Timothy C. “Synthetic, Spectroscopic, and Theoretical Investigations into the Interactions and Detoxification of Nitric Oxide in Biology.” 2012. Web. 15 Jan 2021.

Vancouver:

Berto TC. Synthetic, Spectroscopic, and Theoretical Investigations into the Interactions and Detoxification of Nitric Oxide in Biology. [Internet] [Doctoral dissertation]. University of Michigan; 2012. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/2027.42/96117.

Council of Science Editors:

Berto TC. Synthetic, Spectroscopic, and Theoretical Investigations into the Interactions and Detoxification of Nitric Oxide in Biology. [Doctoral Dissertation]. University of Michigan; 2012. Available from: http://hdl.handle.net/2027.42/96117

University of Kashmir

11. Lone, Mushtaq Ahmad. Studies on complexes of TI(I), Pb(II) and Bi(III)with some potential bioligands.

Degree: Chemistry, 2010, University of Kashmir

URL: http://shodhganga.inflibnet.ac.in/handle/10603/3368

None

Conclusion p. 212-218, References included in chapter

Advisors/Committee Members: Khan, Badruddin.

Subjects/Keywords: Bioinorganic Chemistry; Bioligands; Chemistry

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APA (6^th Edition):

Lone, M. A. (2010). Studies on complexes of TI(I), Pb(II) and Bi(III)with some potential bioligands. (Thesis). University of Kashmir. Retrieved from http://shodhganga.inflibnet.ac.in/handle/10603/3368

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):

Lone, Mushtaq Ahmad. “Studies on complexes of TI(I), Pb(II) and Bi(III)with some potential bioligands.” 2010. Thesis, University of Kashmir. Accessed January 15, 2021. http://shodhganga.inflibnet.ac.in/handle/10603/3368.

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

MLA Handbook (7^th Edition):

Lone, Mushtaq Ahmad. “Studies on complexes of TI(I), Pb(II) and Bi(III)with some potential bioligands.” 2010. Web. 15 Jan 2021.

Vancouver:

Lone MA. Studies on complexes of TI(I), Pb(II) and Bi(III)with some potential bioligands. [Internet] [Thesis]. University of Kashmir; 2010. [cited 2021 Jan 15]. Available from: http://shodhganga.inflibnet.ac.in/handle/10603/3368.

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

Council of Science Editors:

Lone MA. Studies on complexes of TI(I), Pb(II) and Bi(III)with some potential bioligands. [Thesis]. University of Kashmir; 2010. Available from: http://shodhganga.inflibnet.ac.in/handle/10603/3368

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

University of Melbourne

12. NORTH, ANDREA. Rhenium and technetium complexes designed for diagnostic imaging and radiotherapy.

Degree: 2015, University of Melbourne

URL: http://hdl.handle.net/11343/55469

► The detection of hypoxia (low physiological oxygen concentrations) is important for the diagnosis and prognosis of various pathologies including ischaemic stroke and cancer. Nitroaromatic-bearing molecules,… (more)

▼ The detection of hypoxia (low physiological oxygen concentrations) is important for the diagnosis and prognosis of various pathologies including ischaemic stroke and cancer. Nitroaromatic-bearing molecules, particularly 2-nitroimidazoles, demonstrate in vivo reduction and cellular retention. When attached to a radionuclide, nitro-aromatic groups have the potential to non-invasively trace intracellular hypoxia by detection with an imaging modality such as single photon emission computed tomography (SPECT). Selected radioactive isotopes of technetium and rhenium are of interest for diagnostic imaging and radiotherapy. A series of different chelate systems were prepared for coordination to rhenium and technetium with the motivation of producing isostructural radiopharmaceutical agents. The first two systems were devised to act as 99mTc-labelled bioreductive agents for imaging hypoxia with the fac-{M(CO)3}+ (M = Re, 99mTc) core. This included a pyridyl hydrazone-based, [2+1] mixed-ligand binding system incorporating a nitrobenzyl motif, and a picolylamine-derived, tridentate coordination system with a 2-nitroimidazole tether. Promising tracer accumulation was observed for the 99mTc-labelled tridentate complex in mice bearing human renal cell carcinoma. The other novel chelate systems that were developed were based upon coordination to the {MO}3+ (M = Re, 99mTc) fragment. This included a series of asymmetrical and symmetrical, N2S2, tetradentate ligands with a hydrazine-hydrazone or dihydrazide backbone. The unsaturated, tetradentate ligands were designed to be functionalised off the peripheral groups to tether a bioreductive motif or covalently bind a targeting biomolecule. The final chapter describes the preparation of a bis-bidentate series of thio-modified hydrazino nicotinic acid (SHYNIC) chelators to stabilise the {MO}3+ (M = Re, 99mTc) core. These ligands were conjugated to targeting peptides, cRGDfK and Tyr3-octreotate, that bind to receptors that are overexpressed on tumours. Ligands and complexes were characterised by a combination of MS, IR, absorbance and luminescence spectroscopy, 1D and 2D NMR and X-ray crystallography. Of the two nitro-containing systems, the nitroimidazole-bearing tridentate complexes emerged as the best candidates for further investigation as hypoxia targeting agents, with detectable accumulation in hypoxia-induced cells and animal tumour models. The N2S2 tetradentate structures did not form stable complexes of sufficient stability and were not explored further. A comprehensive series of well-characterised, stable rhenium and technetium-99m SHYNIC bis-bidentate systems were synthesised. The success of the novel SHYNIC bis-bidentate series warrants further attention for their translation into the radiopharmaceutical setting as potential imaging and therapeutic agents.

Subjects/Keywords: bioinorganic chemistry; coordination chemistry; technetium-99m; rhenium; radiopharmaceuticals

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APA (6^th Edition):

NORTH, A. (2015). Rhenium and technetium complexes designed for diagnostic imaging and radiotherapy. (Doctoral Dissertation). University of Melbourne. Retrieved from http://hdl.handle.net/11343/55469

Chicago Manual of Style (16^th Edition):

NORTH, ANDREA. “Rhenium and technetium complexes designed for diagnostic imaging and radiotherapy.” 2015. Doctoral Dissertation, University of Melbourne. Accessed January 15, 2021. http://hdl.handle.net/11343/55469.

MLA Handbook (7^th Edition):

NORTH, ANDREA. “Rhenium and technetium complexes designed for diagnostic imaging and radiotherapy.” 2015. Web. 15 Jan 2021.

Vancouver:

NORTH A. Rhenium and technetium complexes designed for diagnostic imaging and radiotherapy. [Internet] [Doctoral dissertation]. University of Melbourne; 2015. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/11343/55469.

Council of Science Editors:

NORTH A. Rhenium and technetium complexes designed for diagnostic imaging and radiotherapy. [Doctoral Dissertation]. University of Melbourne; 2015. Available from: http://hdl.handle.net/11343/55469

Freie Universität Berlin

13. Wende, Christian. On the biological activity of copper and nickel ATCUN and phenanthroline complexes.

Degree: 2016, Freie Universität Berlin

URL: http://dx.doi.org/10.17169/refubium-9420

► A copper(II) and nickel(II) binding ATCUN peptide was synthesized and derivatized with different functional groups. By coupling fluorescent dyes we could show that the corresponding… (more)

▼ A copper(II) and nickel(II) binding ATCUN peptide was synthesized and derivatized with different functional groups. By coupling fluorescent dyes we could show that the corresponding metal complexes exhibit not only effective DNA cleavage activity but also that they can act as redox-sensitive probes. We found that the fluorescence quenching caused by energy transfer can be partially reversed by reduction of the copper(II) center during the DNA cleavage process. Coupling ferrocene to the peptide as a redox-active group, however, should gain access to a self-activating nuclease. However, gel electrophoresis experiments showed that only the combination of two adjacent copper(II) centers in Di(ATCUN) peptides has a positive influence on DNA cleavage and results in activation of the complexes in the absence of a reducing or oxidizing agent. The implementation of additional metal centers could also be achieved by functionalization of the ATCUN peptide with the ligand 1,10-phenanthroline, the copper(II) complex of which is one of the most effective known DNA cleavers. The synthesized copper(II) and nickel(II) complexes were examined not only in terms of their nuclease activity but also their potential as artificial proteases and reagents for lipid peroxidation was investigated, whereby this system is given a wide range of biological applications. Based on the combination of two structural motifs a copper(II) phenanthroline hydrazone complex was synthesized, which should merge the properties of hydrazones with the nuclease activity of copper(II) phenanthrolines. Although the DNA cleavage experiments did not meet the expectations due to the big structural and electronic changes of the phenanthroline scaffold we set a starting point for future investigations of this ligand class. These should also include the study of other possible applications of the versatile features of hydrazones, for example as an antioxidant or antibiotic. Furthermore, in another project based on copper(II) phenanthroline we studied the general impact of substituents in positions 2 and 9 on the DNA cleavage activity. As it is known from the corresponding 2,9-dimethyl derivative (neocuproine) that the steric hindrance of the substituents in the copper(II) complex leads to the loss of the nuclease activity we examined to what extent the lack of the activity is transferable to other substituents. Therefore, further derivatives were synthesized and characterized by CHN analysis, ESI mass spectrometry and X-ray diffraction. Albeit the studied complexes have not achieved the efficiency of the copper(II) phenanthroline complex we could clearly show that the DNA cleavage depends on the nature of the substituents and thus on the complex structure and stability. Advisors/Committee Members: m (gender), Prof. Dr. Nora Kulak (firstReferee), Prof. Dr. Christian Müller (furtherReferee).

Subjects/Keywords: bioinorganic; copper; ATCUN; phenanthroline; DNA; cleavage; 500 Naturwissenschaften und Mathematik::540 Chemie

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APA (6^th Edition):

Wende, C. (2016). On the biological activity of copper and nickel ATCUN and phenanthroline complexes. (Thesis). Freie Universität Berlin. Retrieved from http://dx.doi.org/10.17169/refubium-9420

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):

Wende, Christian. “On the biological activity of copper and nickel ATCUN and phenanthroline complexes.” 2016. Thesis, Freie Universität Berlin. Accessed January 15, 2021. http://dx.doi.org/10.17169/refubium-9420.

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

MLA Handbook (7^th Edition):

Wende, Christian. “On the biological activity of copper and nickel ATCUN and phenanthroline complexes.” 2016. Web. 15 Jan 2021.

Vancouver:

Wende C. On the biological activity of copper and nickel ATCUN and phenanthroline complexes. [Internet] [Thesis]. Freie Universität Berlin; 2016. [cited 2021 Jan 15]. Available from: http://dx.doi.org/10.17169/refubium-9420.

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

Council of Science Editors:

Wende C. On the biological activity of copper and nickel ATCUN and phenanthroline complexes. [Thesis]. Freie Universität Berlin; 2016. Available from: http://dx.doi.org/10.17169/refubium-9420

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

University of Hong Kong

14. 甄肇昌. Bioinorganic chemistry of antimony: interaction of antimonial with biomolecules.

Degree: 2004, University of Hong Kong

URL: http://hdl.handle.net/10722/128642

Subjects/Keywords: Biomolecules; Bioinorganic chemistry.; Antimony.

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APA (6^th Edition):

甄肇昌.. (2004). Bioinorganic chemistry of antimony: interaction of antimonial with biomolecules. (Thesis). University of Hong Kong. Retrieved from http://hdl.handle.net/10722/128642

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

Chicago Manual of Style (16^th Edition):

甄肇昌.. “Bioinorganic chemistry of antimony: interaction of antimonial with biomolecules.” 2004. Thesis, University of Hong Kong. Accessed January 15, 2021. http://hdl.handle.net/10722/128642.

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

MLA Handbook (7^th Edition):

甄肇昌.. “Bioinorganic chemistry of antimony: interaction of antimonial with biomolecules.” 2004. Web. 15 Jan 2021.

Note: this citation may be lacking information needed for this citation format:
Author name may be incomplete

Vancouver:

甄肇昌.. Bioinorganic chemistry of antimony: interaction of antimonial with biomolecules. [Internet] [Thesis]. University of Hong Kong; 2004. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/10722/128642.

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

Council of Science Editors:

甄肇昌.. Bioinorganic chemistry of antimony: interaction of antimonial with biomolecules. [Thesis]. University of Hong Kong; 2004. Available from: http://hdl.handle.net/10722/128642

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

University of Rochester

15. Kleingardner, Jesse G. Biological role and applications of covalent heme attachment to polypeptides.

Degree: PhD, 2014, University of Rochester

URL: http://hdl.handle.net/1802/28322

► Heme is a biological cofactor that performs an array of functions, including electron transfer, redox catalysis, and gas sensing and transport. The ligands and local… (more)

▼ Heme is a biological cofactor that performs an array of functions, including electron transfer, redox catalysis, and gas sensing and transport. The ligands and local environment of the heme group are essential in tuning the properties of the heme to perform in such diverse roles. A subset of heme cofactors, known as hemes c, are covalently ligated to the protein backbone via a CXXCH peptide motif, and are mainly dedicated to performing electron transfer. The research described in this thesis focuses on the ways in which covalent attachment of heme c tunes heme properties relevant to electron transfer. The heme attachment motif is known to promote an out-of-plane distortion of the heme called ruffling. Variants of bacterial cytochromes c from Hydrogenobacter thermophilus and Pseudomonas aeruginosa in which the magnitude of heme ruffling has been altered were analyzed by their paramagnetic NMR shifts, enabling a full description of the influence of ruffling on heme hyperne shifts. The analysis was then used to determine the influence of the length of the heme attachment motif, which covalently binds the heme, on the extent of heme ruffling. The analysis determined that in H. thermophilus cytochrome c, both longer (CX4CH) and shorter (CX1CH) heme attachment motifs enhance the heme ruffling distortion. Increased heme ruffling, measured by the hyperfine NMR shift analysis, correlates to a decreased redox potential of the heme in a number of cytochrome c variants, suggesting that a biological role of the heme attachment motif may be to tune the redox potential of the heme to lower potentials via the heme ruffling distortion. The vibrational profile of the heme attachment motif was also investigated with nuclear resonance vibrational spectroscopy, with implications for understanding how heme covalent attachment optimizes electron transfer through vibrational coupling. Finally, an application of the covalent attachment of heme to a peptide derived from cytochrome c is developed via substitution of cobalt for the heme iron. The resulting cobalt microperoxidase is demonstrated to be a rare example of a hydrogen-evolving electrocatalyst that functions in neutral water using a non-noble metal.

Subjects/Keywords: Bioinorganic chemistry; Catalysis; Cytochrome c; Heme; NMR spectroscopy; NRVS

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APA (6^th Edition):

Kleingardner, J. G. (2014). Biological role and applications of covalent heme attachment to polypeptides. (Doctoral Dissertation). University of Rochester. Retrieved from http://hdl.handle.net/1802/28322

Chicago Manual of Style (16^th Edition):

Kleingardner, Jesse G. “Biological role and applications of covalent heme attachment to polypeptides.” 2014. Doctoral Dissertation, University of Rochester. Accessed January 15, 2021. http://hdl.handle.net/1802/28322.

MLA Handbook (7^th Edition):

Kleingardner, Jesse G. “Biological role and applications of covalent heme attachment to polypeptides.” 2014. Web. 15 Jan 2021.

Vancouver:

Kleingardner JG. Biological role and applications of covalent heme attachment to polypeptides. [Internet] [Doctoral dissertation]. University of Rochester; 2014. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/1802/28322.

Council of Science Editors:

Kleingardner JG. Biological role and applications of covalent heme attachment to polypeptides. [Doctoral Dissertation]. University of Rochester; 2014. Available from: http://hdl.handle.net/1802/28322

University of Toronto

16. Zeer-Wanklyn, Conor Jack. Probing the Link between Ni(II) Binding and GTP Hydrolysis by the Escherichia coli Metal Chaperone HypB.

Degree: 2017, University of Toronto

URL: http://hdl.handle.net/1807/77916

►

Nickel enzymes are virulence factors in some human pathogens. Oftentimes the maturation machinery that forms these enzymes includes a nickel chaperone that is also an… (more)

Subjects/Keywords: Bioinorganic chemistry; Escherichia coli; GTPase; Hydrogenase; Nickel; Nickel enzyme; 0485

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APA (6^th Edition):

Zeer-Wanklyn, C. J. (2017). Probing the Link between Ni(II) Binding and GTP Hydrolysis by the Escherichia coli Metal Chaperone HypB. (Masters Thesis). University of Toronto. Retrieved from http://hdl.handle.net/1807/77916

Chicago Manual of Style (16^th Edition):

Zeer-Wanklyn, Conor Jack. “Probing the Link between Ni(II) Binding and GTP Hydrolysis by the Escherichia coli Metal Chaperone HypB.” 2017. Masters Thesis, University of Toronto. Accessed January 15, 2021. http://hdl.handle.net/1807/77916.

MLA Handbook (7^th Edition):

Zeer-Wanklyn, Conor Jack. “Probing the Link between Ni(II) Binding and GTP Hydrolysis by the Escherichia coli Metal Chaperone HypB.” 2017. Web. 15 Jan 2021.

Vancouver:

Zeer-Wanklyn CJ. Probing the Link between Ni(II) Binding and GTP Hydrolysis by the Escherichia coli Metal Chaperone HypB. [Internet] [Masters thesis]. University of Toronto; 2017. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/1807/77916.

Council of Science Editors:

Zeer-Wanklyn CJ. Probing the Link between Ni(II) Binding and GTP Hydrolysis by the Escherichia coli Metal Chaperone HypB. [Masters Thesis]. University of Toronto; 2017. Available from: http://hdl.handle.net/1807/77916

17. Pirovano, Paolo. High-valent nickel complexes supported by pyridinedicarboxamidate ligands in hydrocarbon oxidation reactions.

Degree: School of Chemistry. Discipline of Chemistry, 2017, Trinity College Dublin

URL: http://hdl.handle.net/2262/82057

► High-valent M=O and M-O-X complexes are hypothesised to be potent oxidising intermediates both in enzymatic and small-molecule catalysis. In contrast to those from groups 6-8,… (more)

▼ High-valent M=O and M-O-X complexes are hypothesised to be potent oxidising intermediates both in enzymatic and small-molecule catalysis. In contrast to those from groups 6-8, oxidants that contain late transition metals (Co, Ni, Cu) are poorly understood. Because of their high reactivity, only a few examples of these compounds have been observed. We have investigated complexes of these metals supported by the dianionic pyridinedicarboxamidate pincer ligands (pyN2Me2 and pyN2iPr2). In particular, we have prepared a series of [NiII(L)(pyN2Me2)] complexes, which were successively oxidised, at low temperature to generate metastable [NiIII(L)(pyN2Me2)] species. These NiIII complexes were characterised by UV-Vis, EPR and XAS spectroscopies, and DFT computations. We probed their oxidising power in reactions with phenols (O-H oxidation) and hydrocarbon substrates (C-H oxidation). The NiIII-OAc species oxidised hydrocarbon substrates with a wide range of C-H bond dissociation energies, from xanthene (BDEC-H = 75.5 kcal/mol) to toluene (BDEC-H= 89 kcal/mol). Kinetic analysis of the reactions revealed them to proceed through a hydrogen atom abstraction mechanism, as evidenced by primary D/H kinetic isotope effects (3.0-3.3) and a linear relationship between reaction rates and the BDEC-H of substrates (Bell-Evans-Polanyi relationship). In terms of reaction rates, NiIII-OAc was shown to be a very powerful oxidising agent, greatly surpassing FeIII-O-X and MnIII-O-X species and rivalling the best hydrogen atom abstractors such as FeIV=O and CuIII-OH compounds. We also obtained indirect evidence for the existence of a transient, highly reactive intermediate, in the reaction of a [NiII(CH3CN)(pyN2iPr2)] precursor with m-CPBA. We observed the formation of decay products, which together with isotopic labelling experiments and DFT calculations, formed proof for the formation of the NiIII-O? species. The main ligand degradation product was an unusual benzoxazine, which derived from hydro- gen atom abstraction from a benzylic C?H group of the supporting ligand. In the final part of the thesis, we began to explore the coordination of pyN2iPr2 to other first row transition metals, in view of probing the effect of varying d electron count and electronegativity on the oxidising reactivity of M-O-X complexes. In particular, we have synthesised and characterised [CoII(CH3CN)(pyN2iPr2)], which will serve as the precursor for high valent oxidants, as well as zinc complexes [ZnII(OAc)(pyN2iPr2)]- and [ZnII(Br)2(HpyN2iPr2)]- . Advisors/Committee Members: McDonald, Aidan.

Subjects/Keywords: Nickel complexes; Hydrocarbon oxidation; Reactive Intermediates; Bioinorganic chemistry; Metal oxo complexes

10 more images…

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APA (6^th Edition):

Pirovano, P. (2017). High-valent nickel complexes supported by pyridinedicarboxamidate ligands in hydrocarbon oxidation reactions. (Thesis). Trinity College Dublin. Retrieved from http://hdl.handle.net/2262/82057

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):

Pirovano, Paolo. “High-valent nickel complexes supported by pyridinedicarboxamidate ligands in hydrocarbon oxidation reactions.” 2017. Thesis, Trinity College Dublin. Accessed January 15, 2021. http://hdl.handle.net/2262/82057.

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

MLA Handbook (7^th Edition):

Pirovano, Paolo. “High-valent nickel complexes supported by pyridinedicarboxamidate ligands in hydrocarbon oxidation reactions.” 2017. Web. 15 Jan 2021.

Vancouver:

Pirovano P. High-valent nickel complexes supported by pyridinedicarboxamidate ligands in hydrocarbon oxidation reactions. [Internet] [Thesis]. Trinity College Dublin; 2017. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/2262/82057.

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

Council of Science Editors:

Pirovano P. High-valent nickel complexes supported by pyridinedicarboxamidate ligands in hydrocarbon oxidation reactions. [Thesis]. Trinity College Dublin; 2017. Available from: http://hdl.handle.net/2262/82057

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

East Carolina University

18. Johnson, Rachel Anne. Utilizing Isothermal Titration Calorimetry to Quantify the Thermodynamics of Cadmium Mimicry: A Comparison to Calcium.

Degree: MS, MS-Chemistry, 2016, East Carolina University

URL: http://hdl.handle.net/10342/5907

► Isothermal titration calorimetry (ITC) is a powerful calorimetric method which can determine all thermodynamic parameters (K, [Delta]H, [Delta]G, and [Delta]S) for a binding event in… (more)

Subjects/Keywords: Isothermal Titration Calorimetry (ITC); Bioinorganic Chemistry; Calorimetry; Thermodynamics; Protein binding

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APA (6^th Edition):

Johnson, R. A. (2016). Utilizing Isothermal Titration Calorimetry to Quantify the Thermodynamics of Cadmium Mimicry: A Comparison to Calcium. (Masters Thesis). East Carolina University. Retrieved from http://hdl.handle.net/10342/5907

Chicago Manual of Style (16^th Edition):

Johnson, Rachel Anne. “Utilizing Isothermal Titration Calorimetry to Quantify the Thermodynamics of Cadmium Mimicry: A Comparison to Calcium.” 2016. Masters Thesis, East Carolina University. Accessed January 15, 2021. http://hdl.handle.net/10342/5907.

MLA Handbook (7^th Edition):

Johnson, Rachel Anne. “Utilizing Isothermal Titration Calorimetry to Quantify the Thermodynamics of Cadmium Mimicry: A Comparison to Calcium.” 2016. Web. 15 Jan 2021.

Vancouver:

Johnson RA. Utilizing Isothermal Titration Calorimetry to Quantify the Thermodynamics of Cadmium Mimicry: A Comparison to Calcium. [Internet] [Masters thesis]. East Carolina University; 2016. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/10342/5907.

Council of Science Editors:

Johnson RA. Utilizing Isothermal Titration Calorimetry to Quantify the Thermodynamics of Cadmium Mimicry: A Comparison to Calcium. [Masters Thesis]. East Carolina University; 2016. Available from: http://hdl.handle.net/10342/5907

19. Wang, Lianke. Réduction catalytique du dioxygène et des protons par des complexes dinucléaires de Fe(II) : Catalytic reduction of dioxygen and protons by dinuclear Fe (II) complexes.

Degree: Docteur es, Chimie inorganique et bio inorganique, 2018, Université Grenoble Alpes (ComUE)

URL: http://www.theses.fr/2018GREAV020

►

Cette thèse a présenté la conception et la synthèse de plusieurs complexes de fer bioinspiré portant des groupes thiolate. Leurs propriétés structurelles, électroniques, magnétiques et… (more)

▼

Cette thèse a présenté la conception et la synthèse de plusieurs complexes de fer bioinspiré portant des groupes thiolate. Leurs propriétés structurelles, électroniques, magnétiques et leur relation ont également été étudiées en utilisant différentes méthodes spectroscopiques en combinaison avec des méthodes computationnelles.Ce manuscrit portait principalement sur leurs propriétés catalytiques ou électrocatalytiques vis-à-vis de la réduction de l'O2. Un complexe non-hème diiron (II) avec un groupe thiol unique a été synthétisé et caractérisé. Le groupe thiol peut être déprotoné par une base pour dériver un complexe de thiolate de fer (II) neutre. Les deux complexes ont montré une forte réactivité vis-à-vis de l'O2 pour donner des complexes diron (III) pontés μ-hydroxo et μ-oxo. Le complexe de fer avec thiol est un catalyseur ORR efficace avec une sélectivité de 100% pour la production de H2O2 en présence d'un agent réducteur à un électron et de protons. Lorsque la catalyse est électrochimiquement entraînée, H2O est le produit principal pendant l'électrocatalyse (~ 14-20% de H2O2). Sur la base du fait que le peroxyde d'hydrogène est généré dans les deux cas (quantitativement ou en 20% en catalyse chimique et électrochimique, respectivement), on peut proposer qu'un intermédiaire commun, le complexe fer-peroxo calculé, soit généré pendant la catalyse . Le mécanisme a été étudié expérimentalement et théoriquement, révélant que le contrôle de la sélectivité provient de l'efficacité du système donneur d'électrons (réduction du potentiel chimique ou appliqué).Un autre complexe asymétrique de diiron (II) avec une unité FeCOCp a également été synthétisé et bien caractérisé dans ses deux formes dans MeCN. Ce complexe de diiron (II) asymétrique est un électrocatalyseur actif pour la production de H2 dans un mécanisme E (ECEC) avec une étape d'activation. Les intermédiaires possibles dans le cycle catalytique ont été générés et caractérisés par différentes spectroscopies. Il convient de noter que le fragment bipyridine dans le ligand agit comme un réservoir d'électrons dans le cycle catalytique.De plus, le premier système d'interconversion thiolate / disulfure à base de fer a été présenté dans ce manuscrit, qui a enrichi la famille de l'interconversion favorisée par le métal entre le thiolate et le disulfure. Intéressant, le système à base de fer a montré non seulement l'interconversion induite par l'hailde, mais aussi les propriétés dépendantes du solvant.Enfin, les complexes mononucléaires de fer (III) -thiolate présentaient un état fondamental de spin intermédiaire intéressant. Les mesures de susceptibilité, les spectres RPE de la poudre cw X et QR et les spectres de Mössbauer en poudre à champ nul ont montré que tous les complexes présentaient une anisotropie magnétique distincte. L'approche théorique a démontré que le principal facteur responsable de l'anisotropie magnétique est le couplage spin-orbite (SOC).

This thesis presented the design and synthesis of several bioinspired iron complexes bearing thiolate groups.…

Advisors/Committee Members: Duboc, Carole (thesis director).

Subjects/Keywords: Chimie bioinorganique; Structure électronique; Catalyse; Bioinorganic chemistry; Electronic structure; Catalysis; 540

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APA (6^th Edition):

Wang, L. (2018). Réduction catalytique du dioxygène et des protons par des complexes dinucléaires de Fe(II) : Catalytic reduction of dioxygen and protons by dinuclear Fe (II) complexes. (Doctoral Dissertation). Université Grenoble Alpes (ComUE). Retrieved from http://www.theses.fr/2018GREAV020

Chicago Manual of Style (16^th Edition):

Wang, Lianke. “Réduction catalytique du dioxygène et des protons par des complexes dinucléaires de Fe(II) : Catalytic reduction of dioxygen and protons by dinuclear Fe (II) complexes.” 2018. Doctoral Dissertation, Université Grenoble Alpes (ComUE). Accessed January 15, 2021. http://www.theses.fr/2018GREAV020.

MLA Handbook (7^th Edition):

Wang, Lianke. “Réduction catalytique du dioxygène et des protons par des complexes dinucléaires de Fe(II) : Catalytic reduction of dioxygen and protons by dinuclear Fe (II) complexes.” 2018. Web. 15 Jan 2021.

Vancouver:

Wang L. Réduction catalytique du dioxygène et des protons par des complexes dinucléaires de Fe(II) : Catalytic reduction of dioxygen and protons by dinuclear Fe (II) complexes. [Internet] [Doctoral dissertation]. Université Grenoble Alpes (ComUE); 2018. [cited 2021 Jan 15]. Available from: http://www.theses.fr/2018GREAV020.

Council of Science Editors:

Wang L. Réduction catalytique du dioxygène et des protons par des complexes dinucléaires de Fe(II) : Catalytic reduction of dioxygen and protons by dinuclear Fe (II) complexes. [Doctoral Dissertation]. Université Grenoble Alpes (ComUE); 2018. Available from: http://www.theses.fr/2018GREAV020

University of Lund

20. Mitra, Mainak. Functional Models for Non-heme Mononuclear Iron Oxygenases.

Degree: 2014, University of Lund

URL: https://lup.lub.lu.se/record/4739502 ; https://portal.research.lu.se/ws/files/5599114/4770823.pdf

► Non-heme mononuclear iron oxygenases catalyze a large number of oxidation reactions in biological systems. The reactions are often proposed to proceed via the intermediacy of… (more)

Subjects/Keywords: Atom and Molecular Physics and Optics; Bioinorganic chemistry; Iron; Oxygenases; Catalysis

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APA (6^th Edition):

Mitra, M. (2014). Functional Models for Non-heme Mononuclear Iron Oxygenases. (Doctoral Dissertation). University of Lund. Retrieved from https://lup.lub.lu.se/record/4739502 ; https://portal.research.lu.se/ws/files/5599114/4770823.pdf

Chicago Manual of Style (16^th Edition):

Mitra, Mainak. “Functional Models for Non-heme Mononuclear Iron Oxygenases.” 2014. Doctoral Dissertation, University of Lund. Accessed January 15, 2021. https://lup.lub.lu.se/record/4739502 ; https://portal.research.lu.se/ws/files/5599114/4770823.pdf.

MLA Handbook (7^th Edition):

Mitra, Mainak. “Functional Models for Non-heme Mononuclear Iron Oxygenases.” 2014. Web. 15 Jan 2021.

Vancouver:

Mitra M. Functional Models for Non-heme Mononuclear Iron Oxygenases. [Internet] [Doctoral dissertation]. University of Lund; 2014. [cited 2021 Jan 15]. Available from: https://lup.lub.lu.se/record/4739502 ; https://portal.research.lu.se/ws/files/5599114/4770823.pdf.

Council of Science Editors:

Mitra M. Functional Models for Non-heme Mononuclear Iron Oxygenases. [Doctoral Dissertation]. University of Lund; 2014. Available from: https://lup.lub.lu.se/record/4739502 ; https://portal.research.lu.se/ws/files/5599114/4770823.pdf

University of Illinois – Urbana-Champaign

21. Hwang, Kevin. Cellular metal ion sensing using DNAzymes.

Degree: PhD, Chemistry, 2016, University of Illinois – Urbana-Champaign

URL: http://hdl.handle.net/2142/90712

► Metal ions are important elements in biology and are involved in numerous reactions essential for maintaining life on earth. Most commonly, metal ions confer their… (more)

▼ Metal ions are important elements in biology and are involved in numerous reactions essential for maintaining life on earth. Most commonly, metal ions confer their role as structural elements or catalytic cofactors within metalloproteins. Metalloproteins comprise more than half of all known proteins and are at the heart of several important biological processes including photosynthesis, respiration, and nitrogen fixation. Another equally important role of metal ions is as signaling molecules. It has been shown that changes in concentrations of calcium, zinc, or copper can trigger downstream signaling effect in neurons. Despite these important functions, high levels of many metal ions, especially transition metal ions, are known to be toxic to cells. Thus, cells have adapted strategies to finely regulate the uptake, storage, and distribution of metal ions within different compartments. The importance of these mechanisms for maintaining metal ion homeostasis within cells and the key role of metal ions in life have been of major interest for years. However, the understanding of these mechanisms and how metal ions play their role is largely unknown in many cases. An important step towards advancing our understanding of metal ions is developing the ability to measure their concentrations in different cellular compartments with accuracy and sensitivity. To achieve this goal, several techniques are available that have greatly advanced our understanding of metal ions. However, current methods suffer from a number of limitations that have slowed progress. Analytical tools such as ICP-MS and AAS, while effective at measuring the cocnentrations of metal ions very sensitively, usually work in bulk and thus are not easily amenable to single cell studies let alone the distribution in different cellular compartments. Moreover, these techniques are often unable to distinguish between different oxidation states of a metal ion or between bound and mobile forms. Techniques based on X-ray absorption, such as X-ray fluorescence microscopy (XFM) can simultaneously detect multiple metal ions and can distinguish between different oxidation states. However, these techniques require the use of highly focused X-ray beams limiting more widespread availability of such techniques. Furthermore, biological samples cannot be examined in a real time manner, and the obtained distribution of metal ions represents only total metal content, without regard to whether the metals are easily exchangeable or are tightly bound, a major factor determining biological activity. To overcome these issues several metal ion sensors have been designed based on either small molecules or proteins with great sensitivities of detection. The use of such sensors has provided great insight into the functions of metal ions. However, as these sensors are usually rationally designed through a trial and error process, it is challenging to generalize the successful designs to sense other metal ions or to meet new desired criteria. DNAzymes, DNA sequences with catalytic… Advisors/Committee Members: Lu, Yi (advisor), Lu, Yi (Committee Chair), Chan, Jefferson (committee member), Murphy, Catherine J (committee member), Suslick, Kenneth S (committee member).

Subjects/Keywords: DNAzymes; metal ion sensing, fluorescent sensors; bioinorganic chemistry

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

APA (6^th Edition):

Hwang, K. (2016). Cellular metal ion sensing using DNAzymes. (Doctoral Dissertation). University of Illinois – Urbana-Champaign. Retrieved from http://hdl.handle.net/2142/90712

Chicago Manual of Style (16^th Edition):

Hwang, Kevin. “Cellular metal ion sensing using DNAzymes.” 2016. Doctoral Dissertation, University of Illinois – Urbana-Champaign. Accessed January 15, 2021. http://hdl.handle.net/2142/90712.

MLA Handbook (7^th Edition):

Hwang, Kevin. “Cellular metal ion sensing using DNAzymes.” 2016. Web. 15 Jan 2021.

Vancouver:

Hwang K. Cellular metal ion sensing using DNAzymes. [Internet] [Doctoral dissertation]. University of Illinois – Urbana-Champaign; 2016. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/2142/90712.

Council of Science Editors:

Hwang K. Cellular metal ion sensing using DNAzymes. [Doctoral Dissertation]. University of Illinois – Urbana-Champaign; 2016. Available from: http://hdl.handle.net/2142/90712

University of Georgia

22. Cheatum, Wren Hilliard. Synthetic analogs of the non-heme iron center in superoxide reductase.

Degree: 2014, University of Georgia

URL: http://hdl.handle.net/10724/25764

► Reactive oxygen species, such as superoxide, are associated with many diseases including cancer, diabetes, and atherosclerosis. In order to protect against the presence of reactive… (more)

Subjects/Keywords: Superoxide; Superoxide reductase; Non-heme iron; Bioinorganic chemistry; synthetic analog

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APA (6^th Edition):

Cheatum, W. H. (2014). Synthetic analogs of the non-heme iron center in superoxide reductase. (Thesis). University of Georgia. Retrieved from http://hdl.handle.net/10724/25764

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):

Cheatum, Wren Hilliard. “Synthetic analogs of the non-heme iron center in superoxide reductase.” 2014. Thesis, University of Georgia. Accessed January 15, 2021. http://hdl.handle.net/10724/25764.

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

MLA Handbook (7^th Edition):

Cheatum, Wren Hilliard. “Synthetic analogs of the non-heme iron center in superoxide reductase.” 2014. Web. 15 Jan 2021.

Vancouver:

Cheatum WH. Synthetic analogs of the non-heme iron center in superoxide reductase. [Internet] [Thesis]. University of Georgia; 2014. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/10724/25764.

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

Council of Science Editors:

Cheatum WH. Synthetic analogs of the non-heme iron center in superoxide reductase. [Thesis]. University of Georgia; 2014. Available from: http://hdl.handle.net/10724/25764

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

Universidade Estadual de Campinas

23. Arruda, Eduardo Guimarães Ratier de, 1990-. Miméticos de metalo-beta-lactamases : influência da esfera de coordenação do ZnII sobre a reatividade e interação com AuI/III: Mimetics of metallo-beta-lactamases : ZnII coordination sphere influence over reactivity and interaction with AuI/III.

Degree: 2019, Universidade Estadual de Campinas

URL: http://repositorio.unicamp.br/jspui/handle/REPOSIP/334507

► Abstract: A systematic study of the first coordination sphere over the reactivity and structure of metallo-beta-lactamase (MBL) monozinc model complexes is reported. Three ZnII complexes… (more)

▼ Abstract: A systematic study of the first coordination sphere over the reactivity and structure of metallo-beta-lactamase (MBL) monozinc model complexes is reported. Three ZnII complexes with the tripodal ligands forming the series [Zn(N-NNN)], [Zn(N-NNS)], and [Zn(N-NNO)] where N-NNX represents the tripodal donor atoms, were investigated regarding their ability to mimic MBL. The tripodal series was inspired by MBL active sites in the respective subclasses, which represents the (His, His, His) Zn1 site present in B1 and B3 subclasses, (His, His, Asp) presented in B3 subclass site and the thiolate presented in B1 and B2 sites. The results were reinforced by DFT and TD-DFT calculations. XAS analysis demonstrated the ZnII electronic deficiency significantly changes in the order [Zn(N-NNS)] < [Zn(N-NNN)] < [Zn(N-NNO)]. This effect directly affects the reactivity over nitrocefin and amoxicillin, observed by the kinetics of hydrolysis, which follows the same trend as the other measurements. NMR spectroscopy revealed that the polarization of carboxylic group in the substrate changes accordingly affecting the hydrolysis kinetic. Our results also demonstrated that not only Lewis acidity is changed by the ligand system but also the softness character of the metal. [Zn(N-NNS)] in particular, is softened by the thiolate, promoting the ligand substitution reaction with solvents and favoring secondary interaction with substrates, not observed for [Zn(N-NNO)]. XRD of the models reveals their similar geometric aspects in comparison to the single-crystal structure of GOB-18 (5K0W) MBL. The interaction of these model complexes with AuI/III complexes was evaluated using 1H NMR and ESI-MS and showed a selective interaction depending on the first coordination sphere and in agreement with Pearson acid-base behavior. The present work demonstrate the ZnII electronic details must be considered in the design of new MBL models and can be used in further aid in the design of new clinically useful MBL inhibitors Advisors/Committee Members: UNIVERSIDADE ESTADUAL DE CAMPINAS (CRUESP), Abbehausen, Camilla, 1979- (advisor), Universidade Estadual de Campinas. Instituto de Química (institution), Programa de Pós-Graduação em Química (nameofprogram), Buffon, Regina (committee member), Corbi, Pedro Paulo (committee member), Ferreira, Ana Maria da Costa (committee member), Bergamini, Fernando Rodrigues Goulart (committee member).

Subjects/Keywords: Química bioinorgânica; Metaloproteínas; Beta-Lactamases; Bioinorganic chemistry; Metalloproteins; Beta-Lactamases

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APA (6^th Edition):

Arruda, Eduardo Guimarães Ratier de, 1. (2019). Miméticos de metalo-beta-lactamases : influência da esfera de coordenação do ZnII sobre a reatividade e interação com AuI/III: Mimetics of metallo-beta-lactamases : ZnII coordination sphere influence over reactivity and interaction with AuI/III. (Thesis). Universidade Estadual de Campinas. Retrieved from http://repositorio.unicamp.br/jspui/handle/REPOSIP/334507

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):

Arruda, Eduardo Guimarães Ratier de, 1990-. “Miméticos de metalo-beta-lactamases : influência da esfera de coordenação do ZnII sobre a reatividade e interação com AuI/III: Mimetics of metallo-beta-lactamases : ZnII coordination sphere influence over reactivity and interaction with AuI/III.” 2019. Thesis, Universidade Estadual de Campinas. Accessed January 15, 2021. http://repositorio.unicamp.br/jspui/handle/REPOSIP/334507.

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

MLA Handbook (7^th Edition):

Arruda, Eduardo Guimarães Ratier de, 1990-. “Miméticos de metalo-beta-lactamases : influência da esfera de coordenação do ZnII sobre a reatividade e interação com AuI/III: Mimetics of metallo-beta-lactamases : ZnII coordination sphere influence over reactivity and interaction with AuI/III.” 2019. Web. 15 Jan 2021.

Vancouver:

Arruda, Eduardo Guimarães Ratier de 1. Miméticos de metalo-beta-lactamases : influência da esfera de coordenação do ZnII sobre a reatividade e interação com AuI/III: Mimetics of metallo-beta-lactamases : ZnII coordination sphere influence over reactivity and interaction with AuI/III. [Internet] [Thesis]. Universidade Estadual de Campinas; 2019. [cited 2021 Jan 15]. Available from: http://repositorio.unicamp.br/jspui/handle/REPOSIP/334507.

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

Council of Science Editors:

Arruda, Eduardo Guimarães Ratier de 1. Miméticos de metalo-beta-lactamases : influência da esfera de coordenação do ZnII sobre a reatividade e interação com AuI/III: Mimetics of metallo-beta-lactamases : ZnII coordination sphere influence over reactivity and interaction with AuI/III. [Thesis]. Universidade Estadual de Campinas; 2019. Available from: http://repositorio.unicamp.br/jspui/handle/REPOSIP/334507

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

Arizona State University

24. Williams, Samuel Garrett. Electrocatalytic Comparison of [FeFe]-Hydrogenases.

Degree: Chemistry, 2020, Arizona State University

URL: http://repository.asu.edu/items/62745

Subjects/Keywords: Chemistry; Biochemistry; Bioinorganic; Electrochemistry; Hydrogenase

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

APA (6^th Edition):

Williams, S. G. (2020). Electrocatalytic Comparison of [FeFe]-Hydrogenases. (Doctoral Dissertation). Arizona State University. Retrieved from http://repository.asu.edu/items/62745

Chicago Manual of Style (16^th Edition):

Williams, Samuel Garrett. “Electrocatalytic Comparison of [FeFe]-Hydrogenases.” 2020. Doctoral Dissertation, Arizona State University. Accessed January 15, 2021. http://repository.asu.edu/items/62745.

MLA Handbook (7^th Edition):

Williams, Samuel Garrett. “Electrocatalytic Comparison of [FeFe]-Hydrogenases.” 2020. Web. 15 Jan 2021.

Vancouver:

Williams SG. Electrocatalytic Comparison of [FeFe]-Hydrogenases. [Internet] [Doctoral dissertation]. Arizona State University; 2020. [cited 2021 Jan 15]. Available from: http://repository.asu.edu/items/62745.

Council of Science Editors:

Williams SG. Electrocatalytic Comparison of [FeFe]-Hydrogenases. [Doctoral Dissertation]. Arizona State University; 2020. Available from: http://repository.asu.edu/items/62745

University of Michigan

25. DeToma, Alaina Sara. Insights on Metal Ions and Misfolded Proteins in Alzheimer's Disease Using Flavonoid Derivatives and X-ray Fluorescence Microscopy.

Degree: PhD, Chemistry, 2013, University of Michigan

URL: http://hdl.handle.net/2027.42/100100

► The incidence of Alzheimer’s disease (AD) worldwide has been accelerating at a staggering rate, demonstrating the need to understand its origins clearly. Misfolded proteins such… (more)

▼ The incidence of Alzheimer’s disease (AD) worldwide has been accelerating at a staggering rate, demonstrating the need to understand its origins clearly. Misfolded proteins such as amyloid-beta have been believed to contribute to the disease. Additionally, it has been suggested that the normal functions and localization of metal ions such as Fe(II/III), Cu(I/II), and Zn(II) could be disrupted in the AD brain. There has been evidence to support the possible interplay between Cu(II) and/or Zn(II) with amyloid-beta-related pathology (i.e., metal–amyloid hypothesis); however, this relationship has yet been to be fully elucidated. A growing interest this possible association with AD pathology has led to new strategies for interrogating the metal– amyloid-beta relationship using small molecule metal chelators. Flavonoids are abundant plant-derived molecules that have been known to bind metal ions and interact with amyloid-beta peptides; however, the synergism of these properties toward metal-associated amyloid-beta has previously received little attention. In this thesis, selected flavonoid derivatives were investigated to formulate a structure-interaction-reactivity relationship among chemical structures, metal ions, and amyloid-beta/metal–amyloid-beta species. The molecules myricetin and luteolin, found in fruits and vegetables, were initially screened and found to influence the reactivity of metal–amyloid-beta species. Building upon these initial observations, the interaction and reactivity of the well-known green tea polyphenol (−)-epigallocatechin-3-gallate (EGCG) were explored at the molecular level through biochemical and biophysical investigations. These findings suggest that metal–amyloid-beta–flavonoid species can be generated and possibly lead to off-pathway aggregation in vitro. We further identified the specific contributions of structural features by synthetic manipulation of the flavonoid framework to aminoisoflavone derivatives. Appropriate tuning of hydrophilic and hydrophobic properties within the structural backbone can modify the balance of metal binding and amyloid-beta interaction, which may account for their reactivity toward amyloid-beta and/or metal–amyloid-beta. Taken together, the studies presented herein demonstrate the utility of flavonoids as a source of structures for direct use and/or synthetic modification from which a structure-interaction-reactivity relationship can be formulated for metal-free and metal-associated amyloid-beta species, which will provide insight into development of chemical tools to uncover the involvement of metal–amyloid species in AD. Advisors/Committee Members: Lim, Mi Hee (committee member), Ramamoorthy, Ayyalusamy (committee member), Pecoraro, Vincent L. (committee member), Garneau-Tsodikova, Sylvie (committee member).

Subjects/Keywords: Bioinorganic Chemistry; Alzheimer's Disease; Neurodegenerative Disease; Flavonoid; Amyloid; Biological Chemistry; Chemistry; Science

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

APA (6^th Edition):

DeToma, A. S. (2013). Insights on Metal Ions and Misfolded Proteins in Alzheimer's Disease Using Flavonoid Derivatives and X-ray Fluorescence Microscopy. (Doctoral Dissertation). University of Michigan. Retrieved from http://hdl.handle.net/2027.42/100100

Chicago Manual of Style (16^th Edition):

DeToma, Alaina Sara. “Insights on Metal Ions and Misfolded Proteins in Alzheimer's Disease Using Flavonoid Derivatives and X-ray Fluorescence Microscopy.” 2013. Doctoral Dissertation, University of Michigan. Accessed January 15, 2021. http://hdl.handle.net/2027.42/100100.

MLA Handbook (7^th Edition):

DeToma, Alaina Sara. “Insights on Metal Ions and Misfolded Proteins in Alzheimer's Disease Using Flavonoid Derivatives and X-ray Fluorescence Microscopy.” 2013. Web. 15 Jan 2021.

Vancouver:

DeToma AS. Insights on Metal Ions and Misfolded Proteins in Alzheimer's Disease Using Flavonoid Derivatives and X-ray Fluorescence Microscopy. [Internet] [Doctoral dissertation]. University of Michigan; 2013. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/2027.42/100100.

Council of Science Editors:

DeToma AS. Insights on Metal Ions and Misfolded Proteins in Alzheimer's Disease Using Flavonoid Derivatives and X-ray Fluorescence Microscopy. [Doctoral Dissertation]. University of Michigan; 2013. Available from: http://hdl.handle.net/2027.42/100100

University of Washington

26. Rees, Julian Avery. Insight into Biological Small-Molecule Activation from Enzymes, Model Complexes, and X-ray Spectroscopy.

Degree: PhD, 2016, University of Washington

URL: http://hdl.handle.net/1773/37058

► This dissertation covers the investigation of biological strategies for activating inert small molecules. Chapters 1 and 2 respectively present an introduction to some notable biological… (more)

Subjects/Keywords: Bioinorganic; Manganese; Nitrogenase; Small Molecule Activation; Spectroscopy; X-ray; Chemistry; Biochemistry; Physical chemistry; chemistry

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

APA (6^th Edition):

Rees, J. A. (2016). Insight into Biological Small-Molecule Activation from Enzymes, Model Complexes, and X-ray Spectroscopy. (Doctoral Dissertation). University of Washington. Retrieved from http://hdl.handle.net/1773/37058

Chicago Manual of Style (16^th Edition):

Rees, Julian Avery. “Insight into Biological Small-Molecule Activation from Enzymes, Model Complexes, and X-ray Spectroscopy.” 2016. Doctoral Dissertation, University of Washington. Accessed January 15, 2021. http://hdl.handle.net/1773/37058.

MLA Handbook (7^th Edition):

Rees, Julian Avery. “Insight into Biological Small-Molecule Activation from Enzymes, Model Complexes, and X-ray Spectroscopy.” 2016. Web. 15 Jan 2021.

Vancouver:

Rees JA. Insight into Biological Small-Molecule Activation from Enzymes, Model Complexes, and X-ray Spectroscopy. [Internet] [Doctoral dissertation]. University of Washington; 2016. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/1773/37058.

Council of Science Editors:

Rees JA. Insight into Biological Small-Molecule Activation from Enzymes, Model Complexes, and X-ray Spectroscopy. [Doctoral Dissertation]. University of Washington; 2016. Available from: http://hdl.handle.net/1773/37058

University of California – Berkeley

27. Olea, Jr., Charles. Chemical Consequences of Heme Distortion and the Role of Heme Distortion in Signal Transduction of H-NOX Proteins.

Degree: Molecular & Cell Biology, 2010, University of California – Berkeley

URL: http://www.escholarship.org/uc/item/6wq9g6mk

► Nitric oxide (NO) signaling in mammals controls important processes such as smooth muscle relaxation and neurotransmission by the activation of soluble guanylate cyclase (sGC). NO… (more)

▼ Nitric oxide (NO) signaling in mammals controls important processes such as smooth muscle relaxation and neurotransmission by the activation of soluble guanylate cyclase (sGC). NO binding to the heme domain of sGC leads to dissociation of the iron-histidine (Fe-His) bond, which is required for enzyme activity. The heme domain of sGC belongs to a larger class of proteins called H-NOX (Heme-Nitric oxide/OXygen) binding domains. H-NOX proteins act as sensors for nitric oxide (NO) or oxygen (O₂). The crystal structure of a H-NOX domain from Thermoanaerobacter tengcongensis (Tt H-NOX) contains one of the most distorted hemes reported to date. In this dissertation, I engineered Tt H-NOX to adopt a flatter heme by mutating a conserved residue in the H-NOX family. Decreasing heme distortion in Tt H-NOX increases affinity for O₂ and decreases the reduction potential of the heme iron. Additionally, flattening the heme is associated with significant shifts at the N-terminus of the protein. These results show a clear link between the heme conformation and Tt H-NOX structure and demonstrate that heme distortion is an important determinant for maintaining biochemical properties in H-NOX proteins.The reduction potential of Tt H-NOX was rationally modulated through mutations of the protein scaffold. The degree of heme distortion is directly correlated with the reduction potential of the heme iron. Inducing planarity in the heme causes overlap of the porphyrin orbitals with the d-orbitals of the iron, leading to increased electron density at the iron, which lowers the reduction potential. Rational design of Tt H-NOX to broaden the reduction potential range and change the function of the protein may potentially be used for further applications.NMR solution structures of H-NOX proteins show a conformational change upon disconnection of the heme and proximal helix. The atomic details of these conformational changes are lacking in the NMR structures, however, especially at the heme pocket. I solved a high-resolution crystal structure of a H-NOX mutant mimicking a broken Fe-His bond. This mutant exhibits specific heme conformational changes and a major N-terminal displacement relative to the wild-type H-NOX protein. Fe-His ligation is ubiquitous in all H-NOX domains, thus the heme and protein conformational changes observed in this study are likely to occur throughout the H-NOX family when NO binding ruptures the Fe-His bond.All mechanistic studies on H-NOX activation have been focused on the response to NO. However, little is known about the sub-class of H-NOX proteins that are predicted to sense O₂. A key question is how these H-NOX proteins respond to O₂ binding. I solved the crystal structure of an unligated mimic of Tt H-NOX at high resolution. When compared to wild-type, which is O<sub>2<sub>-bound, large conformation changes in the protein and heme are…

Subjects/Keywords: Biology, Molecular; Chemistry, Biochemistry; Biochemistry; Bioinorganic Chemistry; Chemical Biology; Signal Transduction; Structural Biology

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

APA (6^th Edition):

Olea, Jr., C. (2010). Chemical Consequences of Heme Distortion and the Role of Heme Distortion in Signal Transduction of H-NOX Proteins. (Thesis). University of California – Berkeley. Retrieved from http://www.escholarship.org/uc/item/6wq9g6mk

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):

Olea, Jr., Charles. “Chemical Consequences of Heme Distortion and the Role of Heme Distortion in Signal Transduction of H-NOX Proteins.” 2010. Thesis, University of California – Berkeley. Accessed January 15, 2021. http://www.escholarship.org/uc/item/6wq9g6mk.

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

MLA Handbook (7^th Edition):

Olea, Jr., Charles. “Chemical Consequences of Heme Distortion and the Role of Heme Distortion in Signal Transduction of H-NOX Proteins.” 2010. Web. 15 Jan 2021.

Vancouver:

Olea, Jr. C. Chemical Consequences of Heme Distortion and the Role of Heme Distortion in Signal Transduction of H-NOX Proteins. [Internet] [Thesis]. University of California – Berkeley; 2010. [cited 2021 Jan 15]. Available from: http://www.escholarship.org/uc/item/6wq9g6mk.

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

Council of Science Editors:

Olea, Jr. C. Chemical Consequences of Heme Distortion and the Role of Heme Distortion in Signal Transduction of H-NOX Proteins. [Thesis]. University of California – Berkeley; 2010. Available from: http://www.escholarship.org/uc/item/6wq9g6mk

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

28. Almotairy, Awatif. Toward dual-action platinum(IV) complexes with bioactive ligands as potent anticancer agents.

Degree: 2020, NUI Galway

URL: http://hdl.handle.net/10379/15796

►

Platinum agents (cisplatin, carboplatin and oxaliplatin) have a crucial role in the treatment of many cancers for several decades. However, they have severe side effects… (more)

▼

Platinum agents (cisplatin, carboplatin and oxaliplatin) have a crucial role in the treatment of many cancers for several decades. However, they have severe side effects and a high number of patients have intrinsic or acquired resistance to platinum-based chemotherapy. The need for new platinum agents with better patient tolerability and improved anti-tumoral efficacy is necessary in order to overcome the side effects of those drugs. Platinum(IV) anticancer drugs are prodrugs, which can not only overcome side effects and the resistance to platinum-based chemotherapy but also lead to enhanced tolerability in patients. It is highlighted that only four platinum(IV) complexes have made it into clinical trials, and three out of these four have failed to show clinical efficacy. The efficacy of platinum(IV) agents depends on the stability, reduction rate, degree of cellular accumulation and which enzymes are targeted. Platinum(II) drugs and bioactive ligands (particularly the ones that have epigenetic activity) can act on various targets with various cellular mechanisms and it would be more appropriate to design them as multi-action platinum(IV) prodrugs. This thesis focuses on the synthesis and characterisation of novel platinum(IV) complexes derived from FDA-approved platinum(II) complexes and bioactive, axial carboxylate ligands. Also explored here are the biological activity, cellular effects and reactions with cellular targets. Chapter one provides an overview of platinum(IV) complexes and examples of various dual-action agents with the history of platinum anticancer therapy. Chapter two examines the design and synthetic strategies employed for the development of novel platinum(IV) prodrugs for carboplatin with the histone deacetylase inhibitor (HDACi) 4-phenylbutyrate (PBA) and three different biologically inactive carboxylic acids. Lower accumulation levels and lower cytotoxicity were observed for the carboplatin platinum(IV) complexes compared to cisplatin. The carboplatin platinum(IV) derivative with PBA and benzoate had a higher cytotoxic activity and HDAC inhibition potency than carboplatin. Chapter three investigates platinum(IV) complexes based on the cisplatin scaffold and PBA in cisplatin-sensitive and cisplatin-resistant ovarian cancer cells (A2780 and A2780cis). Three complexes in this study were more cytotoxic in A2780 and A2790cis ovarian cancer cells than cisplatin and induced cell death pathways leading to apoptosis. In Chapter four new platinum(IV) derivatives of oxaliplatin are described which induced oxidative stress and cytotoxicity. Novel platinum(IV) oxaliplatin derivatives with indole propionic acid were synthesised and studied by various techniques. The monocarboxylated complex with an hydroxido ligand in the second axial position was the most cytotoxic and potent ROS inducer compared with cisplatin and oxaliplatin. Chapter five provides overall conclusions and identifies key areas for future work.

2024-02-13

Advisors/Committee Members: Erxleben, Andrea.

Subjects/Keywords: cancer; chemotherapy; cisplatin; carboplatin; oxaliplatin; platinum(IV); 4-phenylbutyrate; indole propionic acid; Chemistry; Bioinorganic chemistry

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APA (6^th Edition):

Almotairy, A. (2020). Toward dual-action platinum(IV) complexes with bioactive ligands as potent anticancer agents. (Thesis). NUI Galway. Retrieved from http://hdl.handle.net/10379/15796

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):

Almotairy, Awatif. “Toward dual-action platinum(IV) complexes with bioactive ligands as potent anticancer agents.” 2020. Thesis, NUI Galway. Accessed January 15, 2021. http://hdl.handle.net/10379/15796.

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

MLA Handbook (7^th Edition):

Almotairy, Awatif. “Toward dual-action platinum(IV) complexes with bioactive ligands as potent anticancer agents.” 2020. Web. 15 Jan 2021.

Vancouver:

Almotairy A. Toward dual-action platinum(IV) complexes with bioactive ligands as potent anticancer agents. [Internet] [Thesis]. NUI Galway; 2020. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/10379/15796.

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

Council of Science Editors:

Almotairy A. Toward dual-action platinum(IV) complexes with bioactive ligands as potent anticancer agents. [Thesis]. NUI Galway; 2020. Available from: http://hdl.handle.net/10379/15796

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

University of Kansas

29. Massie, Allyssa A. Kinetic and Spectroscopic Investigation of Structural Influences on Hydrogen-atom Transfer Reactivity of N5-Ligated Oxomanganese(IV) Complexes.

Degree: PhD, Chemistry, 2018, University of Kansas

URL: http://hdl.handle.net/1808/29307

► High valent iron- and manganese-oxo intermediates perform important hydrogenatom transfer (HAT) reactions in both biological and synthetic systems. There has been extensive characterization of HAT… (more)

▼ High valent iron- and manganese-oxo intermediates perform important hydrogenatom transfer (HAT) reactions in both biological and synthetic systems. There has been extensive characterization of HAT reactivity of enzymatic and synthetic oxoiron(IV) species, and these complexes have been shown to cleave a wide range of C-H bonds. Although there is no evidence for this type of reactivity by manganese enzymes in nature, several synthetic oxomanganese(IV) species are also capable of activating C-H bonds. However, whereas oxoiron(IV) species have been extensively characterized, the factors that influence HAT reactivity of oxomanganese(IV) species is poorly understood. In an effort to further understand the structure-reactivity relationship of oxomanganese(IV) species, a series of novel oxomanganese(IV) species with subtle perturbations to the equatorial ligand field of the neutral, pentadentate supporting ligand were prepared. Extensive spectroscopic studies, including structural characterization by X-ray absorption spectroscopy (XAS), revealed very minor geometric and electronic structure changes. Kinetic studies of C-H bond containing substrates offered insight into the effects of the ligand perturbations on the reactivity of these oxomanganese(IV) species. Electron donation from the supporting ligand decreases the rate of C-H activation. Conversely, weakening the ligand field through the use of a bulkier ligand dramatically speeds up HAT reactivity, allowing for the reaction with the strong C-H bonds of cyclohexane at rates exceeding that of oxoiron(IV) species with similar ligands. Further, it was discovered that the reaction with cyclohexane could be carried out catalytically in the presence of excess oxidant. The products of catalytic cyclohexane oxidation, cyclohexanol and cyclohexanone, provided evidence of the ability of this oxomanganese(IV) species to perform substrate hydroxylation. Lastly, peroxomanganese(III) species are proposed to be important intermediates in many biological systems. However, in both biological and synthetic systems, the factors that determine the cleavage of the O-O versus Mn-O bonds are not well understood. A novel peroxomanganese(III) species was prepared using electrochemically generated superoxide. The electrochemical reduction of this species was probed to further understand the effects of supporting ligand, which has an amide group trans to the peroxo. Advisors/Committee Members: Jackson, Timothy A (advisor), Barybin, Mikhail V (cmtemember), Blakemore, James D (cmtemember), Caricato, Marco (cmtemember), Allgeier, Alan M (cmtemember).

Subjects/Keywords: Inorganic chemistry; Bioinorganic Chemistry; High-Valent Metal Oxos; Hydrogen Atom Transfer; Manganese

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APA (6^th Edition):

Massie, A. A. (2018). Kinetic and Spectroscopic Investigation of Structural Influences on Hydrogen-atom Transfer Reactivity of N5-Ligated Oxomanganese(IV) Complexes. (Doctoral Dissertation). University of Kansas. Retrieved from http://hdl.handle.net/1808/29307

Chicago Manual of Style (16^th Edition):

Massie, Allyssa A. “Kinetic and Spectroscopic Investigation of Structural Influences on Hydrogen-atom Transfer Reactivity of N5-Ligated Oxomanganese(IV) Complexes.” 2018. Doctoral Dissertation, University of Kansas. Accessed January 15, 2021. http://hdl.handle.net/1808/29307.

MLA Handbook (7^th Edition):

Massie, Allyssa A. “Kinetic and Spectroscopic Investigation of Structural Influences on Hydrogen-atom Transfer Reactivity of N5-Ligated Oxomanganese(IV) Complexes.” 2018. Web. 15 Jan 2021.

Vancouver:

Massie AA. Kinetic and Spectroscopic Investigation of Structural Influences on Hydrogen-atom Transfer Reactivity of N5-Ligated Oxomanganese(IV) Complexes. [Internet] [Doctoral dissertation]. University of Kansas; 2018. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/1808/29307.

Council of Science Editors:

Massie AA. Kinetic and Spectroscopic Investigation of Structural Influences on Hydrogen-atom Transfer Reactivity of N5-Ligated Oxomanganese(IV) Complexes. [Doctoral Dissertation]. University of Kansas; 2018. Available from: http://hdl.handle.net/1808/29307

University of Sydney

30. Schilter, David. Synthesis and DNA-binding of Metallocyclic Architectures .

Degree: 2009, University of Sydney

URL: http://hdl.handle.net/2123/5317

► A new family of cationic N-heterocyclic ligand derivatives was prepared and characterised. Among these compounds are halide salts of the dications [Y(spacer)Y]2+, each of which… (more)

▼ A new family of cationic N-heterocyclic ligand derivatives was prepared and characterised. Among these compounds are halide salts of the dications [Y(spacer)Y]2+, each of which comprise two N heterocyclic donor groups (Y = 4,4′-bipy, pyz, apyz, apym) linked by a conformationally flexible spacer such as (CH2)n, α,α′-xylylene, 2,6-lutidylene or thiabicyclo[3.3.1]nonane-2,6 diyl. The diquaternary halide salts were converted to NO3- and PF6- salts, and interaction of these bridging ligands with labile palladium(II) and platinum(II) precursors afforded several multinuclear complexes. Bis(4,4′-bipyridinium) dications were incorporated into the dinuclear macrocycles [M2(2,2′ bipy)2{4,4′ bipy(CH2)n4,4′-bipy}2]8+ (M = Pd, Pt; n = 4, 6), cis [Pd2Cl4{4,4′ bipy(CH2)34,4′-bipy}2]4+, [Pt2(dppp)2{4,4′-bipy(1,2-xylylene)4,4′-bipy}2]8+ and cis-[Pt2Cl4{4,4′-bipy(1,2-xylylene)4,4′-bipy}2]4+. While bis(pyrazinium) analogues were unreactive towards the palladium(II) and platinum(II) precursors, the doubly deprotonated bis(3 aminopyrazinium) and bis(2 aminopyrimidinium) derivatives served as charge-neutral quadruply-bridging ligands in the complexes [Pt4(2,2′ bipy)4{apyz(CH2)6apyz–2H}2]8+ and [Pt4(2,2′ bipy)4{apym(CH2)5apym–2H}2]8+, both of which feature Pt(II). Pt(II) interactions. Larger species formed when the diamine O,O′-bis(2-aminoethyl)octadeca(ethylene glycol) (PEGda) was treated with cis dinitratopalladium(II) and platinum(II) precursors. The resulting complexes [M(N,N)(PEGda)]2+ (M = Pd, Pt; N,N = 2,2′-bipy, en, tmeda) possessed great size (62 membered chelate rings) and aqueous solubility. DNA-binding studies were conducted with selected complexes in order to investigate the types of interactions these species might participate in. Equimolar mixtures containing either the 16mer duplex DNA D2 or the single strand D2a and palladium(II)/platinum(II) complexes were prepared and analysed by negative-ion ESI MS. Studies of D2/Pd(II) mixtures suggested extensive fragmentation was occuring, and the use of [Pd(tmeda)(PEGda)]2+ and [Pd2(2,2′-bipy)2{4,4′-bipy(CH2)44,4′-bipy}2]8+ resulted in D2 adducts of [Pd(tmeda)]2+ and [4,4′-bipy(CH2)44,4′-bipy]2+, respectively. Decomposition also occurred when D2a was used, although 1 : 1 adducts were observed with [Pd(tmeda)(PEGda)]2+, [Pd(2,2′ bipy)(PEGda)]2+ and [Pd2(2,2′-bipy)2{4,4′-bipy(CH2)44,4′-bipy}2]8+. The low intensities of these adducts indicated that they are unstable towards ESI MS. Analogous ESI-MS experiments using platinum(II) derivatives were performed and, in contrast to those with palladium(II), indicated that the complexes remained largely intact. ESI-MS analysis of D2/Pt(II) mixtures allowed for the detection of 1 : 1 D2 adducts of [Pt(en)(PEGda)]2+, [Pt(tmeda)(PEGda)]2+ and [Pt2(2,2′-bipy)2{4,4′-bipy(CH2)44,4′-bipy}2]8+. Intensities of the adduct ions suggested the greater charge and aryl surface area allow the dinuclear species to bind D2 most strongly. Both [Pt(2,2′-bipy)(Mebipy)2]4+ and [Pt(2,2′ bipy)(NH3)2]2+ gave rise to 1 : 2 adducts of D2, although the latter was…

Subjects/Keywords: bioinorganic chemistry; supramolecular chemistry; DNA recognition

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

APA (6^th Edition):

Schilter, D. (2009). Synthesis and DNA-binding of Metallocyclic Architectures . (Thesis). University of Sydney. Retrieved from http://hdl.handle.net/2123/5317

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):

Schilter, David. “Synthesis and DNA-binding of Metallocyclic Architectures .” 2009. Thesis, University of Sydney. Accessed January 15, 2021. http://hdl.handle.net/2123/5317.

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

MLA Handbook (7^th Edition):

Schilter, David. “Synthesis and DNA-binding of Metallocyclic Architectures .” 2009. Web. 15 Jan 2021.

Vancouver:

Schilter D. Synthesis and DNA-binding of Metallocyclic Architectures . [Internet] [Thesis]. University of Sydney; 2009. [cited 2021 Jan 15]. Available from: http://hdl.handle.net/2123/5317.

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

Council of Science Editors:

Schilter D. Synthesis and DNA-binding of Metallocyclic Architectures . [Thesis]. University of Sydney; 2009. Available from: http://hdl.handle.net/2123/5317

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