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钌修饰的铜绿假单胞菌天青蛋白中的质子耦合电子跳跃

Proton-coupled electron hopping in Ru-modified P. aeruginosa azurin.

作者信息

Warren Jeffrey J, Shafaat Oliver S, Winkler Jay R, Gray Harry B

机构信息

Beckman Institute, California Institute of Technology, Pasadena, CA, 91125, USA.

Department of Chemistry, Simon Fraser University, 8888 University Drive, Burnaby, BC, V5A 1S6, Canada.

出版信息

J Biol Inorg Chem. 2016 Mar;21(1):113-9. doi: 10.1007/s00775-016-1332-4. Epub 2016 Jan 20.

DOI:10.1007/s00775-016-1332-4
PMID:26790882
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC4775413/
Abstract

We constructed two artificial multiple-step electron transfer (hopping) systems based on Pseudomonas aeruginosa azurin where a tyrosine (YOH) is situated between Ru(2,2'-bipyridine)2(imidazole)(histidine) and the native copper site: RuH107YOH109 and RuH124-YOH122. We investigated the rates of Cu(I) oxidation by flash-quench generated Ru(III) over a range of conditions that probed the role of proton-coupled oxidation/reduction of YOH in the reaction. Rates of Cu(I) oxidation were enhanced over single-step electron transfer by factors between 3 and 80, depending on specific scaffold and buffer conditions.

摘要

我们基于铜绿假单胞菌天青蛋白构建了两个人工多步电子转移（跳跃）系统，其中一个酪氨酸（YOH）位于钌（2,2'-联吡啶）2（咪唑）（组氨酸）和天然铜位点之间：RuH107YOH109和RuH124 - YOH122。我们在一系列条件下研究了闪光猝灭产生的Ru(III)氧化Cu(I)的速率，这些条件探究了YOH的质子耦合氧化/还原在反应中的作用。根据特定的支架和缓冲条件，Cu(I)氧化速率比单步电子转移提高了3到80倍。

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