Neutron and Atomic Resolution X-ray Structures of a Lytic Polysaccharide Monooxygenase Reveal Copper-Mediated Dioxygen Binding and Evidence for N-Terminal Deprotonation

被引：50

作者：

Bacik, John-Paul ^{[1
,5
]}

Mekasha, Sophanit ^{[2
]}

Forsberg, Zarah ^{[2
]}

Kovalevsky, Andrey Y. ^{[3
]}

Vaaje-Kolstad, Gustav ^{[2
]}

Eijsink, Vincent G. H. ^{[2
]}

Nix, Jay C. ^{[4
]}

Coates, Leighton ^{[3
]}

Cuneo, Matthew J. ^{[3
]}

Unkefer, Clifford J. ^{[1
]}

Chen, Julian C. -H. ^{[1
]}

机构：

[1] Los Alamos Natl Lab, Biosci Div, Prot Crystallog Stn, Los Alamos, NM 87545 USA

[2] Norwegian Univ Life Sci NMBU, Fac Chem Biotechnol & Food Sci, POB 5003, N-1430 As, Norway

[3] Oak Ridge Natl Lab, Biol & Soft Matter Div, 1 Bethel Valley Rd,POB 2008, Oak Ridge, TN 37831 USA

[4] Lawrence Berkeley Lab, Adv Light Source, 1 Cyclotron Rd, Berkeley, CA 94720 USA

[5] Princeton Univ, Dept Chem, Princeton, NJ 08544 USA

来源：

BIOCHEMISTRY | 2017年 / 56卷 / 20期

关键词：

FUNCTIONAL-CHARACTERIZATION; ACTIVE-SITE; CELLULOSE; DEGRADATION; CHITIN; CRYSTALLOGRAPHY; COORDINATION; ACTIVATION; HISTIDINE; CU(II);

D O I：

10.1021/acs.biochem.7b00019

中图分类号：

Q5 [生物化学]; Q7 [分子生物学];

学科分类号：

070307 [化学生物学]; 071010 [生物化学与分子生物学];

摘要：

A 1.1 angstrom resolution, room-temperature X-ray structure and a 2.1 angstrom resolution neutron structure of a chitin-degrading lytic polysaccharide monooxygenase domain from the bacterium Jonesia denitrificans (IdLPM010A) show a putative dioxygen species equatorially bound to the active site copper. Both structures show an elongated density for the dioxygen, most consistent with a Cu(II)-bound peroxide. The coordination environment is consistent with Cu(II). In the neutron and X-ray structures, difference maps reveal the N-terminal amino group, involved in copper coordination, is present as a mixed ND2 and ND-, suggesting a role for the copper ion in shifting the pK(a) of the amino terminus.

引用

页码：2529 / 2532

页数：4

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