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Title: Chemical and biosynthetic studies of chlorophylls

Thesis/Dissertation ·
OSTI ID:6983944

Chlorophyll occurrence, structure, biosynthesis, and degradation are discussed. Degradation and ring cleavage of heme is also discussed. The author examines the formation of dihydrobiliverdins by alkaline hydrolysis of zinc(II) meso-trifluoroacetoxypheophoribides, as a possible model for chlorophyll catabolism. {sup 18}O{sub 2}-labelling experiments show that the dihydrobiliverdin terminal lactam oxygens are derived from two different dioxygen molecules, also analogous to the Two Oxygen Molecular mechanism observed in heme degradation. The initially obtained dihydrobiliverdin readily undergoes an isomeric structural transformation, which is proposed as a model for the P{sub R}-P{sub FR} interconversion of the light sensor pigment phytochrome. The generality of the ring-opening reaction is demonstrated with various chlorophyll-derived zinc(II) trifluoroacetoxychlorins, and side reactions of the isocyclic ring are discussed. The synthesis and properties of a chlorophyll-derived meso-oxochlorin are described. Facile one-electron oxidation, and its inhibition by protonation, is demonstrated by NMR, ESR, and cyclic voltammetry studies. Cyclic voltammetry is also used to measure redox potentials of a range of pheophorbide and meso-trifluoroacetoxypheophorbide metal complexes, including an oxochlorin nickel(II) complex. The results are presented of biosynthetic feeding studies of green sulfur bacteria with {sup 13}C- and {sup 14}C-labelled glutamate, glycine, and methionine. This study examines an unusual oxidation of a bacteriomethylpheophorbide 5-ethyl substituent, and describes attempts to elucidate the mechanism by {sup 18}O-labelling studies. Attempts to similarily derivatize a pyropheophorbide 5-methyl substituent are discussed.

Research Organization:
California Univ., Davis, CA (USA)
OSTI ID:
6983944
Resource Relation:
Other Information: Thesis (Ph. D.)
Country of Publication:
United States
Language:
English