The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases

Frandsen, Kristian E H; Simmons, Thomas J; Dupree, Paul; Poulsen, Jens-Christian N; Hemsworth, Glyn R; Ciano, Luisa; Johnston, Esther M; Tovborg, Morten; Johansen, Katja S; von Freiesleben, Pernille; Marmuse, Laurence; Fort, S�bastien; Cottaz, Sylvain; Driguez, Hugues; Henrissat, Bernard; Lenfant, Nicolas; Tuna, Floriana; Baldansuren, Amgalanbaatar; Davies, Gideon J; Lo Leggio, Leila; Walton, Paul H

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.

Citation

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., Lo Leggio, L., & 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

• Journal Article Type: Article
• Acceptance Date: Jan 12, 2016
• Online Publication Date: Feb 29, 2016
• Publication Date: 2016-04
• Deposit Date: Feb 13, 2020
• Journal: Nature Chemical Biology
• Print ISSN: 1552-4450
• Electronic ISSN: 1552-4469
• Publisher: Nature Publishing Group
• Peer Reviewed: Peer Reviewed
• Volume: 12
• Issue: 4
• Pages: 298-303
• DOI: https://doi.org/10.1038/nchembio.2029
• Public URL: https://nottingham-repository.worktribe.com/output/3829537
• Publisher URL: https://www.nature.com/articles/nchembio.2029
• Additional Information: Received: 24 September 2015; Accepted: 12 January 2016; First Online: 29 February 2016; : M.T. and P.v.F. are employees of Novozymes, a producer of enzymes for industrial use.