Structural and electronic determinants of lytic polysaccharide monooxygenase reactivity on polysaccharide substrates.
Structural and electronic determinants of lytic polysaccharide monooxygenase reactivity on polysaccharide substrates.
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DOI：
10.1038/s41467-017-01247-3
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发表时间：
2017-10-20
影响因子：
16.6
通讯作者：
Dupree P
中科院分区：
文献类型：
--
作者：
Simmons TJ;Frandsen KEH;Ciano L;Tryfona T;Lenfant N;Poulsen JC;Wilson LFL;Tandrup T;Tovborg M;Schnorr K;Johansen KS;Henrissat B;Walton PH;Lo Leggio L;Dupree P
裂解性多糖单加氧酶（LPMO）是工业上重要的铜依赖性酶，其氧化裂解多糖。在这里，我们提出了两个密切相关的AA 9家族LPMO的功能和结构表征相似香菇（LsAA 9A）和Collariella virescens（CvAA 9A）。LsAA 9A和CvAA 9A裂解一系列多糖，包括纤维素、木葡聚糖、混合键葡聚糖和葡甘露聚糖。LsAA 9A另外切割分离的木聚糖底物。CvAA 9A和LsAA 9A结合到纤维素和非纤维素寡糖的结构提供了对其特异性的分子决定因素的深入了解。光谱测量揭示了木聚糖和葡聚糖结合后铜配位的差异。LsAA 9A活性在切割木聚糖时对还原剂电位不太敏感，表明木聚糖和葡聚糖切割存在不同的催化机制。总之，这些数据表明，AA 9 LPMO可以显示不同的表观底物特异性，这取决于结合表面上的生产性蛋白质-碳水化合物相互作用以及铜活性位点处的电子因素。铜依赖性溶解性多糖单加氧酶（LPM 0）氧化裂解多糖。在这里，作者提出了真菌LPMO的结构-功能表征，表明特定的LPMO使用涉及替代铜配位几何结构的机制切割木聚糖。
Lytic polysaccharide monooxygenases (LPMOs) are industrially important copper-dependent enzymes that oxidatively cleave polysaccharides. Here we present a functional and structural characterization of two closely related AA9-family LPMOs from Lentinus similis (LsAA9A) and Collariella virescens (CvAA9A). LsAA9A and CvAA9A cleave a range of polysaccharides, including cellulose, xyloglucan, mixed-linkage glucan and glucomannan. LsAA9A additionally cleaves isolated xylan substrates. The structures of CvAA9A and of LsAA9A bound to cellulosic and non-cellulosic oligosaccharides provide insight into the molecular determinants of their specificity. Spectroscopic measurements reveal differences in copper co-ordination upon the binding of xylan and glucans. LsAA9A activity is less sensitive to the reducing agent potential when cleaving xylan, suggesting that distinct catalytic mechanisms exist for xylan and glucan cleavage. Overall, these data show that AA9 LPMOs can display different apparent substrate specificities dependent upon both productive protein–carbohydrate interactions across a binding surface and also electronic considerations at the copper active site. Copper-dependent lytic polysaccharide monooxygenases (LPMOs) oxidatively cleave polysaccharides. Here the authors present a structure-function characterization of fungal LPMOs, showing that a particular LPMO cleaves xylan using a mechanism that involves an alternative copper coordination geometry.
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影响因子：
4.4
作者：
Kojima Y;Várnai A;Ishida T;Sunagawa N;Petrovic DM;Igarashi K;Jellison J;Goodell B;Alfredsen G;Westereng B;Eijsink VG;Yoshida M
通讯作者：
Yoshida M
DOI：
10.1107/s0907444904019158
发表时间：
2004-12-01
影响因子：
2.2
作者：
Emsley, P;Cowtan, K
通讯作者：
Cowtan, K
DOI：
10.1073/pnas.1323629111
发表时间：
2014-04-29
影响因子：
11.1
作者：
Agger, Jane W.;Isaksen, Trine;Westereng, Bjorge
通讯作者：
Westereng, Bjorge
影响因子：
6.3
作者：
Fanuel M;Garajova S;Ropartz D;McGregor N;Brumer H;Rogniaux H;Berrin JG
通讯作者：
Berrin JG
影响因子：
3.1
作者：
Lenfant, Nicolas;Hainaut, Matthieu;Henrissat, Bernard
通讯作者：
Henrissat, Bernard