Gated electron transfer of cytochrome c6 at biomimetic interfaces: a time-resolved SERR study

被引：21

作者：

Kranich, Anja ^{[1
]}

Naumann, Hendrik ^{[1
]}

Molina-Heredia, Fernando P. ^{[2
,3
]}

Moore, H. Justin ^{[4
]}

Lee, T. Randall ^{[4
]}

Lecomte, Sophie ^{[5
]}

de la Rosa, Miguel A. ^{[2
,3
]}

Hildebrandt, Peter ^{[1
]}

Murgida, Daniel H. ^{[6
]}

机构：

[1] Tech Univ Berlin, Inst Chem, D-10623 Berlin, Germany

[2] Univ Seville, Inst Bioquim Vegetal & Fotosintesis, Ctr Invest Cient Isla Cartuja, Seville, Spain

[3] CSIC, E-41080 Seville, Spain

[4] Univ Houston, Dept Chem, Houston, TX 77204 USA

[5] Univ Bordeaux 1, CNRS, CBMN, UMR5248, F-33607 Pessac, France

[6] Univ Buenos Aires, Fac Ciencias Exactas & Nat, Dept Quim Inorgan Analit & Quim Fis, INQUIMAE CONICET, Buenos Aires, DF, Argentina

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2009年 / 11卷 / 34期

关键词：

PHOTOSYSTEM-I REDUCTION; RESONANCE RAMAN-SPECTROSCOPY; REDOX-COUPLED PROCESSES; PCC; 7119; REACTION-MECHANISM; TRANSIENT COMPLEX; COATED ELECTRODES; GOLD ELECTRODES; HEME-PROTEINS; PLASTOCYANIN;

D O I：

10.1039/b904434e

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The electron shuttle heme protein Cyt-c(6) from the photosynthetic cyanobacterium Nostoc sp. PCC 7119 was immobilized on nanostructured Ag electrodes coated with SAMs that mimic different possible interactions with its natural reaction partner PSI. The structure, redox potential, and electron-transfer dynamics of the SAM-Cyt-c(6) complexes were investigated by TR-SERR spectroelectrochemistry. It is shown that the heterogeneous electron-transfer process is gated both in electrostatic and hydrophobic-hydrophilic complexes. At long tunneling distances, the reaction rate is controlled by the tunneling probability, while at shorter distances or higher driving forces, protein dynamics becomes the rate-limiting event.

引用

页码：7390 / 7397

页数：8

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