Preparation, Characterization, and Oxygenase Activity of a Photocatalytic Artificial Enzyme

被引：29

作者：

Gu, Yifan ^{[1
]}

Ellis-Guardiola, Ken ^{[1
]}

Srivastava, Poonam ^{[1
]}

Lewis, Jared C. ^{[1
]}

机构：

[1] Univ Chicago, Dept Chem, Chicago, IL 60637 USA

来源：

CHEMBIOCHEM | 2015年 / 16卷 / 13期

基金：

美国国家科学基金会;

关键词：

artificial enzymes; oxygenases; photocatalysts; prolyl oligopeptidases; unnatural amino acids; HYPERTHERMOPHILE PYROCOCCUS-FURIOSUS; PROLYL OLIGOPEPTIDASE; ELECTRON-TRANSFER; CONFORMATIONAL-CHANGES; ORGANIC-SYNTHESIS; SINGLET OXYGEN; DBD DYES; EVOLUTION; ENERGY; MECHANISM;

D O I：

10.1002/cbic.201500165

中图分类号：

Q5 [生物化学]; Q7 [分子生物学];

学科分类号：

071010 ; 081704 ;

摘要：

A bicyclo[6,1,0]nonyne-substituted 9-mesityl-10-methyl-acridinium cofactor was prepared and covalently linked to a prolyl oligopeptidase scaffold containing a genetically encoded 4-azido-L-phenylalanine residue in its active site. The resulting artificial enzyme catalyzed sulfoxidation when irradiated with visible light in the presence of air. This reaction proceeds by initial electron abstraction from the sulfide within the enzyme active site, and the protein scaffold extended the fluorescence lifetime of the acridium cofactor. The mode of sulfide activation and placement of the acridinium cofactor (5) in POP-ZA(4)-5 make this artificial enzyme a promising platform for developing selective photocatalytic transformations.

引用

页码：1880 / 1883

页数：4

共 33 条

[1]

[Anonymous], 2008, ANGEW CHEM

[2]

[Anonymous], 1996, SULFUR REP, DOI DOI 10.1080/01961779608047906

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