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Electron hopping through proteins

Warren, Jeffrey J. and Ener, Maraia E. and Vlček, Antonín, Jr. and Winkler, Jay R. and Gray, Harry B. (2012) Electron hopping through proteins. Coordination Chemistry Reviews , 256 (21-22). pp. 2478-2487. ISSN 0010-8545 . PMCID PMC3570191. http://resolver.caltech.edu/CaltechAUTHORS:20121116-101610363

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Abstract

Biological redox machines require efficient transfer of electrons and holes for function. Reactions involving multiple tunneling steps, termed “hopping,” often promote charge separation within and between proteins that is essential for energy storage and conversion. Here we show how semiclassical electron transfer theory can be extended to include hopping reactions: graphical representations (called hopping maps) of the dependence of calculated two-step reaction rate constants on driving force are employed to account for flow in a rhenium-labeled azurin mutant as well as in two structurally characterized redox enzymes, DNA photolyase and MauG. Analysis of the 35 Å radical propagation in ribonucleotide reductases using hopping maps shows that all tyrosines and tryptophans on the radical pathway likely are involved in function. We suggest that hopping maps can facilitate the design and construction of artificial photosynthetic systems for the production of fuels and other chemicals.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1016/j.ccr.2012.03.032DOIArticle
http://www.sciencedirect.com/science/article/pii/S0010854512000768PublisherArticle
https://www.ncbi.nlm.nih.gov/pmc/articles/PMC3570191PubMed CentralArticle
ORCID:
AuthorORCID
Winkler, Jay R.0000-0002-4453-9716
Additional Information:© 2012 Elsevier B.V. Received 17 December 2011; Accepted 30 March 2012; Available online 5 April 2012. Our work is supported by NIH (DK019038 to H.B.G. and J.R.W.; GM095037 to J.J.W.), an NSF Center for Chemical Innovation (Powering the Planet, CHE-0947829) and by a Czech Ministry of Education Grant ME10124 to A.V. This article belongs to a special issue "Solar Fuels- by invitation only," edited By Tony Vlcek.
Group:CCI Solar Fuels
Funders:
Funding AgencyGrant Number
NIHDK019038
NIHGM095037
NSFCHE-0947829
Ministry of Education (Czech Republic)ME10124
Subject Keywords:Electron transfer; Multistep tunneling; Hopping maps; Redox proteins azurin; Ribonucleotide reductase; DNA photolyase; MauG
PubMed Central ID:PMC3570191
Record Number:CaltechAUTHORS:20121116-101610363
Persistent URL:http://resolver.caltech.edu/CaltechAUTHORS:20121116-101610363
Official Citation:Jeffrey J. Warren, Maraia E. Ener, Antonín Vlček Jr., Jay R. Winkler, Harry B. Gray, Electron hopping through proteins, Coordination Chemistry Reviews, Volume 256, Issues 21–22, November 2012, Pages 2478-2487, ISSN 0010-8545, 10.1016/j.ccr.2012.03.032.
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:35511
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:20 Nov 2012 19:49
Last Modified:26 Jul 2017 22:19

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