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Concerted bond switching mechanism coupled with one-electron transfer for the oxygen-oxygen bond formation in the oxygen-evolving complex of photosystem II
Chemical Physics Letters ( IF 2.8 ) Pub Date : 2018-10-17 , DOI: 10.1016/j.cplett.2018.10.041
Mitsuo Shoji , Hiroshi Isobe , Kizashi Yamaguchi

We here precisely analyzed the electronic structures during the oxygen-oxygen (O-O) bond formation of the oxygen-evolving complex (OEC) in photosystem II (PSII) based on the quantum mechanics/molecular mechanics (QM/MM) calculations. Changes in the spin density and the chemical indices derived from the natural orbitals suggested that the O(5)-O(6) bond formation proceeds with a concerted bond breaking of the Mn4-O(5) coupled with the through-bond one-electron transfer from the O(6) site to the Mn4 site (Mn4(IV) -> Mn4(III)). This mechanism can be best described as a Concerted Bond Switching (CBS) mechanism, which is a non-radical reaction of the O(5)-O(6) bond formation.



中文翻译:

协同键转换机制与单电子转移相结合,在光系统II的析氧复合物中形成氧-氧键

我们在此基于量子力学/分子力学(QM / MM)计算,精确分析了光系统II(PSII)中的放氧配合物(OEC)的氧-氧(OO)键形成过程中的电子结构。自旋密度和源自自然轨道的化学指数的变化表明,O (5) -O (6)键的形成与Mn 4 -O (5)的键合协同断裂以及贯穿键结合一起进行电子从O (6)位置转移到Mn 4位置(Mn 4(IV)-> Mn 4(III))。此机制可以最好地描述为协调键转换(CBS)机制,它是O (5) -O (6)键形成的非自由基反应。

更新日期:2018-10-17
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