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 Sébastien, Cottaz Sylvain, Driguez Hugues, Henrissat Bernard, Lenfant Nicolas, Tuna Floriana, Baldansuren Amgalanbaatar, Davies Gideon J, Lo Leggio Leila, Walton Paul H
Department of Chemistry, University of Copenhagen, Copenhagen, Denmark.
Department of Biochemistry, University of Cambridge, Cambridge, UK.
Nat Chem Biol. 2016 Apr;12(4):298-303. doi: 10.1038/nchembio.2029. Epub 2016 Feb 29.
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.
裂解多糖单加氧酶（LPMOs）是一类含铜酶，可氧化分解诸如纤维素和几丁质等难降解多糖。自被发现以来，LPMOs已成为生物质工业利用中的重要因素，尤其是在纤维素生物乙醇的可持续生产方面。我们在此报告了一种LPMO-寡糖复合物的结构测定结果，从而对这些酶的作用机制有了详细的了解。通过结合结构和电子顺磁共振光谱，我们揭示了LPMOs与糖类底物相互作用的方式。我们进一步揭示了酶活性位点的电子和结构特征，展示了LPMOs如何协调氧气与多糖链的反应。
