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First-Principles Study on Structural and Chemical Asymmetry of a Biomimetic Water-Splitting Dimanganese Complex
Zhou, Ting1; Lin, Xiangsong2,3; Zheng, Xiao1,4
Source PublicationJOURNAL OF CHEMICAL THEORY AND COMPUTATION
2013-02-01
DOI10.1021/ct301034j
Volume9Issue:2Pages:1073-1080
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical ; Physics, Atomic, Molecular & Chemical
WOS Research AreaChemistry ; Physics
WOS KeywordOXYGEN-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
AbstractDensity-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.
Language英语
WOS IDWOS:000315018300024
Citation statistics
Cited Times:7[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/137720
Collection中国科学院大连化学物理研究所
Affiliation1.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
GB/T 7714
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.
APA Zhou, Ting,Lin, Xiangsong,&Zheng, Xiao.(2013).First-Principles Study on Structural and Chemical Asymmetry of a Biomimetic Water-Splitting Dimanganese Complex.JOURNAL OF CHEMICAL THEORY AND COMPUTATION,9(2),1073-1080.
MLA Zhou, Ting,et al."First-Principles Study on Structural and Chemical Asymmetry of a Biomimetic Water-Splitting Dimanganese Complex".JOURNAL OF CHEMICAL THEORY AND COMPUTATION 9.2(2013):1073-1080.
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