Axial Ligation of Heme in c-Type Cytochromes of Living Shewanella oneidensis: A New Insight into Enhanced Extracellular Electron Transfer

文献类型： 外文期刊

第一作者： Yuan, Yong

作者： Yuan, Yong;Zhou, Shungui;Li, Laicai

作者机构：

关键词： axial ligation;c-type cytochromes;density functional calculations;extracellular electron transfer;Shewanella oneidensis

期刊名称：CHEMELECTROCHEM （ 影响因子：4.59； 五年影响因子：4.509 ）

ISSN： 2196-0216

年卷期： 2015 年 2 卷 11 期

页码：

收录情况： SCI

摘要： The controlled axial ligation reaction of the heme Fe in c-type cytochromes (c-Cyts) is a valid approach to regulating the redox activity of c-Cyts, but it is mainly revealed in purified c-Cyts. Herein, we demonstrate the first example of regulating the redox activity of c-Cyts in a living microorganism through heme axial ligation to target high extracellular electron transfer (EET). The direct electrochemistry of Shewanella oneidensis amended with an axial ligand (imidazole) delivered a 1.5-fold increase in the biocurrent, demonstrating enhanced EET. Invivo UV/Vis and Raman spectra confirmed the axial ligation of imidazoles to the c-Cyts. Density functional calculations revealed the optimized electronic structure and lowered reorganization energy values of the imidazole-ligated heme, which benefited EET. These findings provide, not only a better understanding of the mechanism underlying the EET, but also new insights into the enhanced EET.

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