The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Abstract

Lytic polysaccharide monooxygenases (LPMOs) are copper-containing enzymes that oxidatively break down recalcitrant polysaccharides such as cellulose and chitin. Since their discovery, LPMOs have become integral factors in the industrial utilization of biomass, especially in the sustainable generation of cellulosic bioethanol. We report here a structural determination of an LPMO-oligosaccharide complex, yielding detailed insights into the mechanism of action of these enzymes. Using a combination of structure and electron paramagnetic resonance spectroscopy, we reveal the means by which LPMOs interact with saccharide substrates. We further uncover electronic and structural features of the enzyme active site, showing how LPMOs orchestrate the reaction of oxygen with polysaccharide chains.

Metadata

Item Type:	Article
Authors/Creators:	Frandsen, Kristian E H Simmons, Thomas J Dupree, Paul Poulsen, Jens-Christian N. Hemsworth, Glyn Robert https://orcid.org/0000-0002-8226-1380 Ciano, Luisa https://orcid.org/0000-0002-1667-0856 Johnston, Esther Michelle (ej716@york.ac.uk) Tovborg, Morten Johansen, Katja Salomon von Freiesleben, Pernille Marmuse, Laurence Fort, Sébastien Cottaz, Sylvain Driguez, Hugues Henrissat, Bernard Lenfant, Nicolas Tuna, Floriana Baldansuren, Amgalanbaatar Davies, Gideon John https://orcid.org/0000-0002-7343-776X Lo Leggio, Leila Walton, Paul Howard https://orcid.org/0000-0002-1152-1480
Copyright, Publisher and Additional Information:	© 2016 Nature America, Inc. All rights reserved. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details
Keywords:	Amino Acid Sequence,Aspergillus oryzae/enzymology,Binding Sites,Catalytic Domain,Cellulose/metabolism,Chitin/metabolism,Copper/metabolism,Crystallography, X-Ray,Fluorescence Resonance Energy Transfer,Lentinula/enzymology,Mixed Function Oxygenases/chemistry,Models, Molecular,Molecular Sequence Data,Oligosaccharides/chemistry,Oxidation-Reduction,Substrate Specificity
Dates:	Published: 1 April 2016 Published (online): 29 February 2016 Accepted: 12 January 2016
Institution:	The University of York
Academic Units:	The University of York > Faculty of Sciences (York) > Chemistry (York)
Depositing User:	Pure (York)
Date Deposited:	05 Apr 2016 14:45
Last Modified:	25 Dec 2024 00:13
Published Version:	https://doi.org/10.1038/nchembio.2029
Status:	Published
Refereed:	Yes
Identification Number:	10.1038/nchembio.2029
Related URLs:	http://www.scopus.com/inward/record.url?... http://www.nature.com/nchembio/journal/v...
Open Archives Initiative ID (OAI ID):	oai:eprints.whiterose.ac.uk:97868

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The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

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