Artificial metalloenzymes as catalysts for oxidative lignin degradation
Date
05/11/2018Author
Grant ID
EP/J018139/1
EP/J018139/1
SUBICAT
657755
Metadata
Show full item recordAbstract
We report novel artificial metalloenzymes (ArMs), containing tris(pyridylmethyl)amine (TPA), for the atom economic oxidation of lignin β-O-4 model compounds, using hydrogen peroxide. The protein scaffold alters the selectivity of the reaction from a low yielding cleavage reaction when using the parent Fe-tpa complex to a high yielding benzylic alcohol oxidation when using the complex incorporated into a protein scaffold, SCP-2L A100C. Engineering the protein scaffold to incorporate glutamic acid was found to improve the ArM activity, showing that rational design of the protein environment using metal binding amino acids can be a first step towards improving the overall activity of an artificial metalloenzyme.
Citation
Doble , M , Jarvis , A , Ward , A , Colburn , J D , Goetze , J P , Buehl , M & Kamer , P C J 2018 , ' Artificial metalloenzymes as catalysts for oxidative lignin degradation ' , ACS Sustainable Chemistry & Engineering , vol. 6 , no. 11 , pp. 15100-15107 . https://doi.org/10.1021/acssuschemeng.8b03568
Publication
ACS Sustainable Chemistry & Engineering
Status
Peer reviewed
ISSN
2168-0485Type
Journal article
Rights
Copyright © 2018 American Chemical Society. This work has been made available online in accordance with the publisher’s policies. This is the author created accepted version manuscript following peer review and as such may differ slightly from the final published version. The final published version of this work is available at https://doi.org/10.1021/acssuschemeng.8b03568
Description
M.V.D thanks the BBSRC for support through an EastBio studentship BB/J01446X/1. The authors thank the EPSRC for funding through the EPSRC critical mass grant “Clean catalysis for sustainable development” (EP/J018139/1). This work was supported by the EU the European Union (Marie Curie ITN “SuBiCat” PITN-GA-2013-60704 (P.C.J.K), and through a Marie Curie Individual Fellowship project ArtOxiZymes to A.G.J. (H2020-MSCA-IF-2014- 657755). A.G.J would also like to thank the University of Edinburgh for funding through a Christina Miller Fellowship. The UK Catalysis Hub is kindly thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium, which is funded by the EPSRC (EP/K014706/2, EP/K014668/1, EP/K014854/1, EP/K014714/1, and EP/M013219/1).Collections
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