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题名: First-Principles Study on Structural and Chemical Asymmetry of a Biomimetic Water-Splitting Dimanganese Complex
作者: Zhou, Ting1;  Lin, Xiangsong2, 3;  Zheng, Xiao1, 4
刊名: JOURNAL OF CHEMICAL THEORY AND COMPUTATION
发表日期: 2013-02-01
DOI: 10.1021/ct301034j
卷: 9, 期:2, 页:1073-1080
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical ;  Physics, Atomic, Molecular & Chemical
研究领域[WOS]: Chemistry ;  Physics
英文摘要: Density-functional theory calculations are carried out for a biomimetic dimanganese complex, [H2O(terpy)-Mn-III(mu-O)(2)Mn-IV(terpy)OH2](3+)(1, terpy = 2,2':6',2 ''-terpyridine), which is a structural model for the oxygen evolving center of photosystem II. Theoretical investigations aim at elucidating the asymmetry features in the geometric and electronic structures of complex 1, as well as their influences on the chemical functions of the two manganese centers, in the presence of water solvent. With the insight gained from the first-principles calculations, we study the oxidation state of complex 1 in the acetate buffer solution. Both the thermodynamic and kinetic aspects are explored in detail, and the structural and chemical asymmetry of the two manganese centers is fully considered. It is found that the larger steric repulsion associated with the Mn(IV) center plays a decisive role, which leads to the predominant acetate coordination at the Mn(III) ion. This thus resolves the existing controversy on the preferential acetate binding to complex 1.
关键词[WOS]: OXYGEN-EVOLVING COMPLEX ;  O BOND FORMATION ;  CORRELATED MOLECULAR CALCULATIONS ;  GAUSSIAN-BASIS SETS ;  MU-OXO MIMICS ;  PHOTOSYSTEM-II ;  O-2 EVOLUTION ;  ARTIFICIAL PHOTOSYNTHESIS ;  HYSCORE SPECTROSCOPY ;  ANGSTROM RESOLUTION
语种: 英语
WOS记录号: WOS:000315018300024
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/137720
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Univ Sci & Technol China, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, Ctr Theoret Computat Chem, Dalian 116023, Peoples R China
4.Guizhou Normal Coll, Inst Appl Phys, Guizhou Prov Key Lab Computat Nanomat Sci, Guiyang 550018, Guizhou, Peoples R China

Recommended Citation:
Zhou, Ting,Lin, Xiangsong,Zheng, Xiao. First-Principles Study on Structural and Chemical Asymmetry of a Biomimetic Water-Splitting Dimanganese Complex[J]. JOURNAL OF CHEMICAL THEORY AND COMPUTATION,2013,9(2):1073-1080.
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