Quantum Refinement Does Not Support Dinuclear Copper Sites in Crystal Structures of Particulate Methane Monooxygenase.
Quantum Refinement Does Not Support Dinuclear Copper Sites in Crystal Structures of Particulate Methane Monooxygenase.
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DOI：
10.1002/anie.201708977
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发表时间：
2018-01-02
期刊：
影响因子：
--
通讯作者：
Ryde U
中科院分区：
文献类型：
--
作者：
Cao L;Caldararu O;Rosenzweig AC;Ryde U
颗粒甲烷单加氧酶(PMMO)是为数不多的能够激活甲烷的酶之一。这种酶的金属含量一直备受争议，有人认为它可能是双核Fe中心，也可能是单、双或三核铜中心。晶体结构显示了一个单核或双核的铜中心，但分辨率较低，并且双核中心的几何形状不寻常。我们使用了量子精化(用量子力学计算增强的晶学精化)来改善活性中心的结构。我们比较了一些不同的单核和双核几何结构，在某些情况下，用更多的蛋白质配体或一两个水分子来增强，以确定哪种结构最适合两组结晶学原始数据。在所有情况下，单核铜中心的效果最好，偶尔也会有额外的水分子。因此，我们得出结论，在pMMO中不存在双核铜中心的结晶学支撑。用量子精细方法研究了颗粒甲烷单加氧酶(PMMO)的两种晶体结构。对于假定的活性中心，比较了几种不同的单核和双核几何构型，在某些情况下具有更多的蛋白质配体或一两个水分子，以确定哪种结构最符合结晶学原始数据。结果表明，在pMMO中没有双核铜中心的晶体支撑。
Particulate methane monooxygenase (pMMO) is one of the few enzymes that can activate methane. The metal content of this enzyme has been highly controversial, with suggestions of a dinuclear Fe site or mono-, di-, or trinuclear Cu sites. Crystal structures have shown a mono- or dinuclear Cu site, but the resolution was low and the geometry of the dinuclear site unusual. We have employed quantum refinement (crystallographic refinement enhanced with quantum-mechanical calculations) to improve the structure of the active site. We compared a number of different mono- and dinuclear geometries, in some cases enhanced with more protein ligands or one or two water molecules, to determine which structure fits the two sets of crystallographic raw data best. In all cases, the best results were obtained with mononuclear Cu sites, occasionally with an extra water molecule. Thus we conclude that there is no crystallographic support for a dinuclear Cu site in pMMO. Two crystal structures of particulate methane monooxygenase (pMMO) were studied with quantum refinement. For the putative active site, several different mono- and dinuclear geometries, in some cases with more protein ligands or one or two water molecules, were compared to determine which structure fits the crystallographic raw data best. The results indicate that there is no crystallographic support for a dinuclear Cu site in pMMO.
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影响因子：
15
作者：
Martinho, Marlene;Choi, Dong W.;Muenck, Eckard
通讯作者：
Muenck, Eckard
DOI：
10.1073/pnas.0536703100
发表时间：
2003-04-01
影响因子：
11.1
作者：
Lieberman, RL;Shrestha, DB;Rosenzweig, AC
通讯作者：
Rosenzweig, AC
DOI：
10.1107/s0907444911035918
发表时间：
2012-04-01
期刊：
ACTA CRYSTALLOGRAPHICA SECTION D-BIOLOGICAL CRYSTALLOGRAPHY
影响因子：
--
作者：
Tickle, Ian J.
通讯作者：
Tickle, Ian J.
影响因子：
15
作者：
Yoshizawa, Kazunari;Shiota, Yoshihito
通讯作者：
Shiota, Yoshihito
影响因子：
62.1
作者：
Solomon, Edward I.;Heppner, David E.;Johnston, Esther M.;Ginsbach, Jake W.;Cirera, Jordi;Qayyum, Munzarin;Kieber-Emmons, Matthew T.;Kjaergaard, Christian H.;Hadt, Ryan G.;Tian, Li
通讯作者：
Tian, Li