Large-scale QM/MM calculations of the CaMn4O5 cluster in the S3 state of the oxygen evolving complex of photosystem II. Comparison between water-inserted and no water-inserted structures

被引：29

作者：

Shoji, Mitsuo ^{[1
,2
]}

Isobe, Hiroshi ^{[3
]}

Nakajima, Takahito ^{[4
]}

Shigeta, Yasuteru ^{[1
,2
]}

Suga, Michihiro ^{[3
]}

Akita, Fusamichi ^{[3
]}

Shen, Jian-Ren ^{[3
]}

Yamaguchi, Kizashi ^{[4
,5
,6
]}

机构：

[1] Univ Tsukuba, Ctr Computat Sci, Tennodai 1-1-1, Tsukuba, Ibaraki 3058577, Japan

[2] Univ Tsukuba, Grad Sch Pure & Appl Sci, Tennodai 1-1-1, Tsukuba, Ibaraki 3058577, Japan

[3] Okayama Univ, Grad Sch Nat Sci & Technol, Res Inst Interdisciplinary Sci, Okayama, Okayama 7008530, Japan

[4] Riken Adv Inst Computat Sci, Kobe, Hyogo 6500047, Japan

[5] Osaka Univ, Inst NanoSci Design, Toyonaka, Osaka 5608531, Japan

[6] Handairigaku Technores NPO, Toyonaka, Osaka 5600043, Japan

来源：

FARADAY DISCUSSIONS | 2017年 / 198卷

关键词：

DINUCLEAR RUTHENIUM COMPLEX; O BOND FORMATION; CRYSTAL-STRUCTURE; ELECTRON-TRANSFER; CHEMICAL-BONDS; OXIDATION CHEMISTRY; PROTON RELEASE; MECHANISM; TRANSITION; EXCHANGE;

D O I：

10.1039/c6fd00230g

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

Large-scale QM/MM calculations were performed to elucidate an optimized geometrical structure of a CaMn4O5 cluster with and without water insertion in the S-3 state of the oxygen evolving complex (OEC) of photosystem II (PSII). The left (L)-opened structure was found to be stable under the assumption of no hydroxide anion insertion in the S-3 state, whereas the right (R)-opened structure became more stable if one water molecule is inserted to the Mn4Ca cluster. The optimized Mn-a(4)-Mn-d(1) distance determined by QM/MM was about 5.0 angstrom for the S-3 structure without an inserted hydroxide anion, but this is elongated by 0.2-0.3 angstrom after insertion. These computational results are discussed in relation to the possible mechanisms of O-O bond formation in water oxidation by the OEC of PSII.

引用

页码：83 / 106

页数：24

共 17 条

[1] Large-scale QM/MM calculations of the CaMn4O5 cluster in the oxygen-evolving complex of photosystem II: Comparisons with EXAFS structures
Shoji, Mitsuo
Isobe, Hiroshi
Nakajima, Takahito
Yamaguchi, Kizashi
CHEMICAL PHYSICS LETTERS, 2016, 658 : 354 - 363
[2] Theoretical illumination of water-inserted structures of the CaMn4O5 cluster in the S2 and S3 states of oxygen-evolving complex of photosystem II: full geometry optimizations by B3LYP hybrid density functional
Isobe, H.
Shoji, M.
Yamanaka, S.
Umena, Y.
Kawakami, K.
Kamiya, N.
Shen, J. -R.
Yamaguchi, K.
DALTON TRANSACTIONS, 2012, 41 (44) : 13727 - 13740
[3] Generalized approximate spin projection calculations of effective exchange integrals of the CaMn4O5 cluster in the S1 and S3 states of the oxygen evolving complex of photosystem II
Isobe, H.
Shoji, M.
Yamanaka, S.
Mino, H.
Umena, Y.
Kawakami, K.
Kamiya, N.
Shen, J. -R.
Yamaguchi, K.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 2014, 16 (24) : 11911 - 11923
[4] Geometric, electronic and spin structures of the CaMn4O5 catalyst for water oxidation in oxygen-evolving photosystem II. Interplay between experiments and theoretical computations
Yamaguchi, Kizashi
Shoji, Mitsuo
Isobe, Hiroshi
Kawakami, Takashi
Miyagawa, Koichi
Suga, Michihiro
Akita, Fusamichi
Shen, Jian-Ren
COORDINATION CHEMISTRY REVIEWS, 2022, 471
[5] Theoretical studies of the damage- free S1 structure of the CaMn4O5 cluster in oxygen-evolving complex of photosystem II
Shoji, Mitsuo
Isobe, Hiroshi
Yamanaka, Shusuke
Suga, Michihiro
Akita, Fusamichi
Shen, Jian-Ren
Yamaguchi, Kizashi
CHEMICAL PHYSICS LETTERS, 2015, 623 : 1 - 7
[6] On the guiding principles for lucid understanding of the damage-free S1 structure of the CaMn4O5 cluster in the oxygen evolving complex of photosystem II
Center for Computational Sciences, University of Tsukuba, Tsukuba, Ibaraki
305-8577, Japan
不详
700-8530, Japan
不详
560-0043, Japan
不详
560-8531, Japan
不详
560-0043, Japan
Chem. Phys. Lett., (44-52):
[7] On the guiding principles for lucid understanding of the damage-free S1 structure of the CaMn4O5 cluster in the oxygen evolving complex of photosystem II
Shoji, Mitsuo
Isobe, Hiroshi
Yamanaka, Shusuke
Suga, Michihiro
Akita, Fusamichi
Shen, Jian-Ren
Yamaguchi, Kizashi
CHEMICAL PHYSICS LETTERS, 2015, 627 : 44 - 52
[8] Large-Scale QM/MM Calculations of Hydrogen Bonding Networks for Proton Transfer and Water Inlet Channels for Water Oxidation-Theoretical System Models of the Oxygen-Evolving Complex of Photosystem II
Shoji, M.
Isobe, H.
Yamanaka, S.
Umena, Y.
Kawakami, K.
Kamiya, N.
Shen, J-R
Nakajima, T.
Yamaguchi, K.
ADVANCES IN QUANTUM CHEMISTRY, VOL 70, 2015, 70 : 325 - 413
[9] The nature of chemical bonds of the CaMn4O5 cluster in oxygen evolving complex of photosystem II: Jahn-Teller distortion and its suppression by Ca doping in cubane structures
Yamaguchi, K.
Yamanaka, S.
Isobe, H.
Saito, T.
Kanda, K.
Umena, Y.
Kawakami, K.
Shen, J. -R.
Kamiya, N.
Okumura, M.
Nakamura, H.
Shoji, M.
Yoshioka, Y.
INTERNATIONAL JOURNAL OF QUANTUM CHEMISTRY, 2013, 113 (04) : 453 - 473
[10] On the guiding principles for understanding of geometrical structures of the CaMn4O5 cluster in oxygen-evolving complex of photosystem II. Proposal of estimation formula of structural deformations via the Jahn-Teller effects
Yamaguchi, K.
Shoji, M.
Isobe, H.
Yamanaka, S.
Umena, Y.
Kawakami, K.
Kamiya, N.
MOLECULAR PHYSICS, 2017, 115 (05) : 636 - 666

← 1 2 →