Oriented immobilization of Desulfovibrio gigas hydrogenase onto carbon electrodes by covalent bonds for nonmediated oxidation of H2

被引:135
作者
Rüdiger, O
Abad, JM
Hatchikian, EC
Fernandez, VM
De Lacey, AL
机构
[1] CSIC, Inst Catalisis, Madrid 28049, Spain
[2] CNRS, Inst Biol Struct & Microbiol, F-13402 Marseille, France
关键词
D O I
10.1021/ja0554312
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The orientation of hydrogenase bound covalently to a pyrolytic graphite edge electrode modified with a 4-aminophenyl monolayer can be modulated via electrostatic interactions during the immobilization step. At low ionic strength and when the amino groups of the electrode surface are mostly protonated, the hydrogenase is immobilized with the negatively charged region that surrounds its 4Fe4S cluster nearer to the protein surface facing the electrode. This allows direct electron transfer between the immobilized hydrogenase and the electrode, which is observed by the strong catalytic currents measured in the presence of the H2 substrate. Therefore, a very stable enzymatic electrode is produced that catalyzes nonmediated H2 oxidation. Copyright © 2005 American Chemical Society.
引用
收藏
页码:16008 / 16009
页数:2
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