The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Kristian E H Frandsen; Thomas J Simmons; Paul Dupree; Jens-Christian N. Poulsen; Glyn Robert Hemsworth; Luisa Ciano; Esther Michelle Johnston; Morten Tovborg; Katja Salomon Johansen; Pernille von Freiesleben; Laurence Marmuse; Sébastien Fort; Sylvain Cottaz; Hugues Driguez; Bernard Henrissat; Nicolas Lenfant; Floriana Tuna; Amgalanbaatar Baldansuren; Gideon John Davies; Leila Lo Leggio; Paul Howard Walton

doi:10.1038/nchembio.2029

The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Kristian E H Frandsen, Thomas J Simmons, Paul Dupree, Jens-Christian N. Poulsen, Glyn Robert Hemsworth, Luisa Ciano, Esther Michelle Johnston, Morten Tovborg, Katja Salomon Johansen, Pernille von Freiesleben, Laurence Marmuse, Sébastien Fort, Sylvain Cottaz, Hugues Driguez, Bernard Henrissat, Nicolas Lenfant, Floriana Tuna, Amgalanbaatar Baldansuren, Gideon John Davies, Leila Lo LeggioPaul Howard Walton

Chemistry

Research output: Contribution to journal › Article › peer-review

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.

Original language	English
Pages (from-to)	298–303
Number of pages	6
Journal	NATURE CHEMICAL BIOLOGY
Volume	12
Issue number	4
Early online date	29 Feb 2016
DOIs	https://doi.org/10.1038/nchembio.2029
Publication status	Published - 1 Apr 2016

Bibliographical note

© 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

Access to Document

10.1038/nchembio.2029

Walton_manuscript_peer_reviewed
© 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.
Accepted author manuscript, 939 KBLicence: Unspecified

http://www.nature.com/nchembio/journal/v12/n4/full/nchembio.2029.html

Cite this

Frandsen, K. E. H., Simmons, T. J., Dupree, P., Poulsen, J.-C. N., Hemsworth, G. R., Ciano, L., Johnston, E. M., Tovborg, M., Johansen, K. S., von Freiesleben, P., Marmuse, L., Fort, S., Cottaz, S., Driguez, H., Henrissat, B., Lenfant, N., Tuna, F., Baldansuren, A., Davies, G. J., ... Walton, P. H. (2016). The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases. NATURE CHEMICAL BIOLOGY, 12(4), 298–303. https://doi.org/10.1038/nchembio.2029

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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.",

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Frandsen, KEH, Simmons, TJ, Dupree, P, Poulsen, J-CN, Hemsworth, GR , Ciano, L , Johnston, EM, Tovborg, M, Johansen, KS, von Freiesleben, P, Marmuse, L, Fort, S, Cottaz, S, Driguez, H, Henrissat, B, Lenfant, N, Tuna, F, Baldansuren, A, Davies, GJ, Lo Leggio, L & Walton, PH 2016, 'The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases', NATURE CHEMICAL BIOLOGY, vol. 12, no. 4, pp. 298–303. https://doi.org/10.1038/nchembio.2029

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The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Abstract

Bibliographical note

Keywords

Access to Document

Other files and links

Gideon John Davies, FRS, FMedSci

Paul Howard Walton

Molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Polysaccharide cleavage by LPMO AA9 family

Cite this

The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Abstract

Bibliographical note

Keywords

Access to Document

Other files and links

Profiles

Gideon John Davies, FRS, FMedSci

Paul Howard Walton

Activities

Molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Datasets

Polysaccharide cleavage by LPMO AA9 family

Cite this