The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases.

The molecular basis of polysaccharide cleavage by lytic polysaccharide monooxygenases.
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溶解性多糖单加氧酶裂解多糖的分子基础。

DOI:
10.1038/nchembio.2029
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发表时间:
2016-04
影响因子:
14.8
通讯作者:
Walton PH
Walton PH
中科院分区:
生物学1区
文献类型:
--
作者:
Frandsen KE;Simmons TJ;Dupree P;Poulsen JC;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

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裂解多糖单加氧酶 (LPMO) 是一种含铜酶,可氧化分解纤维素和甲壳素等顽固多糖。自发现以来,LPMO 已成为生物质工业利用中不可或缺的因素,特别是在纤维素生物乙醇的可持续生产中。我们在此报告了 LPMO-低聚糖复合物的首次结构测定,从而详细了解了这些酶的作用机制。通过结合结构和电子顺磁共振波谱,我们揭示了 LPMO 与糖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 LPMO 如何协调氧与多糖链的反应。
Lytic polysaccharide monooxygenases (LPMOs) are copper-containing enzymes which 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 the first 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.