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Insights into structure and redox potential of lignin peroxidase from QM/MM calculations

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Buhl_2016_OBC_Insights_CCBY.pdf (769.1Kb)
Date
28/02/2016
Author
Castro, Ludovic
Crawford, Luke
Mutengwa, Archford
Goetze, Jan Philipp
Buehl, Michael
Keywords
QD Chemistry
DAS
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Abstract
Redox potentials are computed for the active form (compound I) of lignin peroxidase (LiP) using a suitable QM/MM methodology (B3LYP/SDD/6-311G**//BP86/SVP:CHARMM). Allowing for dynamic conformational averaging, a potential of 0.67(33) V relative to ferrocenium/ferrocene is obtained for the active form with its oxoiron(IV) core. The computed redox potential is very sensitive to the charge distribution around the active site: protonation of titratable residues close to the metal center increases the redox potential, thereby rationalising the known pH dependence of LiP activity. A simple MM-charge deletion scheme is used to identify residues that are critical for the redox potential. Two mutant proteins are studied through homology modelling, E40Q and D183N, which are predicted to have an increased redox potential by 140 mV and 190 mV, respectively, relative to the wild type. These mutant proteins are thus promising targets for synthesis and further exploration toward a rational design of biocatalytic systems for oxidative degradation of lignin.
Citation
Castro , L , Crawford , L , Mutengwa , A , Goetze , J P & Buehl , M 2016 , ' Insights into structure and redox potential of lignin peroxidase from QM/MM calculations ' , Organic & Biomolecular Chemistry , vol. 14 , no. 8 , pp. 2385-2389 . https://doi.org/10.1039/C6OB00037A
Publication
Organic & Biomolecular Chemistry
Status
Peer reviewed
DOI
https://doi.org/10.1039/C6OB00037A
ISSN
1477-0520
Type
Journal article
Rights
Copyright 2016 the Authors. This article is licensed under a Creative Commons Attribution 3.0 Unported Licence (http://creativecommons.org/licenses/by/3.0/).
Description
The authors wish to thank EaStCHEM, the School of Chemistry and the EPSRC (grant code EP/J018139/1) for funding
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  • University of St Andrews Research
URL
http://www.rsc.org/suppdata/c6/ob/c6ob00037a/c6ob00037a1.pdf
URI
http://hdl.handle.net/10023/8473

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