期刊
BIOCHEMISTRY
卷 52, 期 44, 页码 7703-7706出版社
AMER CHEMICAL SOC
DOI: 10.1021/bi401214v
关键词
-
资金
- Division of Chemical Sciences, Geosciences, and Biosciences, Office of Basic Energy Sciences, U.S. Department of Energy [DESC0001423]
- Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences [DE-FG02-05ER15646]
- Computational Materials and Chemical Sciences (CMCSN) project at Brookhaven National Laboratory [DE-AC02-98CH10886]
- U.S. DOE
- Division of Chemical Sciences, Geosciences & Biosciences, Office of Basic Energy Sciences
The S-0 -> S-1 transition of the oxygen-evolving complex (OEC) of photosystem II is one of the least understood steps in the Kok cycle of water splitting. We introduce a quantum mechanics/molecular mechanics (QM/MM) model of the S-0 state that is consistent with extended X-ray absorption fine structure spectroscopy and X-ray diffraction data. In conjunction with the QM/MM model of the S-1 state, we address the proton-coupled electron-transfer (PCET) process that occurs during the S-0 -> S-1 transition, where oxidation of a Mn center and deprotonation of a mu-oxo bridge lead to a significant rearrangement in the OEC. A hydrogen bonding network, linking the D1-D61 residue to a Mn-bound water molecule, is proposed to facilitate the PCET mechanism.
作者
我是这篇论文的作者
点击您的名字以认领此论文并将其添加到您的个人资料中。
推荐
暂无数据