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Freie Universität Berlin

1. Mößler, Johann. Synthesis, Spectroscopic Characterization and Electron Transfer Properties of Covalently Linked Chlorin- and Bacteriochlorin-Quinones as Model Compounds for Photosynthesis.

Degree: 1999, Freie Universität Berlin

This dissertation describes the synthesis and electron transfer properties of covalently linked biomimetic diads, containing a chlorin or a bacteriochlorin as electron donor and p-benzoquinone as electron aceptor. Two meso-substituted chlorin-quinones, linked via the chlorin-positions 5 and 10, and a bacteriochlorin-quinone were obtained by reduction of a porphyrin- hydroquinone with diimine, followed by selective oxidation of the hydroquinone moiety with p – benzoquinone. Semiempirical calculations of the LCAO-pz-coefficients, based on the results from EPR/ENDOR experiments on cation and anion radicals of (bacterio)chlorins and diads, predict a high efficient charge separation in a chlorin-quinone linked via the chlorin-position 10. Time-resolved fluorescence spectroscopy in dichloromethane and toluene on 1,4 -trans-cyclohexylene-linked diads show a strong dependency of the singulet electron transfer rate on the free enthalpy of electron transfer, while the LCAO-pz-coefficients at the linking positions seem to have only little influence on kET. It is assumed that the electron transfer takes place mainly through the solvent. The electron transfer in the free bases of these chlorin- and bacteriochlorin-quinones ist about five times faster than in the corresponding porphyrin-quinone. The charge-separated state tends to be more long-lived in chlorin-quinones linked via chlorin-position 10, confirming the predictions from the semiempirical calculations in part. Time-resolved triplet EPR spectra show spin polarization patterns similar to natural chlorophylls. The kinetics of the triplet electron transfer were studied on a cyclohexylene-linked Zn(II)-chlorin-quinone in ethanol glass matrix at 130 K. Advisors/Committee Members: n (gender), Prof. Dr. Harry Kurreck (firstReferee), Prof. Dr. Jürgen-Hinrich Fuhrhop (furtherReferee), Prof. Dr. Hans-Heinrich Limbach, Prof. Dr. Klaus Christmann (furtherReferee).

Subjects/Keywords: Porphyrins; Bacteriochlorins; Quinones; Photosynthesis; Electron Transfer; Biomimetic; 500 Naturwissenschaften und Mathematik::540 Chemie::540 Chemie und zugeordnete Wissenschaften

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APA (6th Edition):

Mößler, J. (1999). Synthesis, Spectroscopic Characterization and Electron Transfer Properties of Covalently Linked Chlorin- and Bacteriochlorin-Quinones as Model Compounds for Photosynthesis. (Thesis). Freie Universität Berlin. Retrieved from http://dx.doi.org/10.17169/refubium-8451

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

Chicago Manual of Style (16th Edition):

Mößler, Johann. “Synthesis, Spectroscopic Characterization and Electron Transfer Properties of Covalently Linked Chlorin- and Bacteriochlorin-Quinones as Model Compounds for Photosynthesis.” 1999. Thesis, Freie Universität Berlin. Accessed August 13, 2020. http://dx.doi.org/10.17169/refubium-8451.

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

MLA Handbook (7th Edition):

Mößler, Johann. “Synthesis, Spectroscopic Characterization and Electron Transfer Properties of Covalently Linked Chlorin- and Bacteriochlorin-Quinones as Model Compounds for Photosynthesis.” 1999. Web. 13 Aug 2020.

Vancouver:

Mößler J. Synthesis, Spectroscopic Characterization and Electron Transfer Properties of Covalently Linked Chlorin- and Bacteriochlorin-Quinones as Model Compounds for Photosynthesis. [Internet] [Thesis]. Freie Universität Berlin; 1999. [cited 2020 Aug 13]. Available from: http://dx.doi.org/10.17169/refubium-8451.

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

Council of Science Editors:

Mößler J. Synthesis, Spectroscopic Characterization and Electron Transfer Properties of Covalently Linked Chlorin- and Bacteriochlorin-Quinones as Model Compounds for Photosynthesis. [Thesis]. Freie Universität Berlin; 1999. Available from: http://dx.doi.org/10.17169/refubium-8451

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

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