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Theoretical study of iron acyl complexes modeling the active site of [Fe]-hydrogenase: Solvation effects play a significant role
Li, Chaozheng1,2; Fu, Zhiqiang2,3; Zhang, Xiaoqian1; Liu, Yufang1; Wang, Yong2
KeywordDensity Functional Theoretical Calculation Solvation Effects Iron Transition State Exothermic Process
Source PublicationCOMPUTATIONAL AND THEORETICAL CHEMISTRY
2015-07-15
DOI10.1016/j.comptc.2015.04.014
Volume1064Pages:45-50
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Physical Sciences
WOS SubjectChemistry, Physical
WOS Research AreaChemistry
WOS KeywordCLUSTER-FREE HYDROGENASE ; H-2-FORMING METHYLENETETRAHYDROMETHANOPTERIN DEHYDROGENASE ; DENSITY-FUNCTIONAL THERMOCHEMISTRY ; METAL-FREE HYDROGENASE ; FE-ONLY HYDROGENASE ; CYTOCHROME-P450 CATALYZED-REACTIONS ; CRYSTAL-STRUCTURE ; METHANOGENIC ARCHAEA ; DESULFOVIBRIO-DESULFURICANS ; LIGHT-INACTIVATION
AbstractIn this work, density functional theory (DFT) calculations were carried out to study the role of solvation effects on the reaction of diiron dithiolate complex with CO to form [Fe]-hydrogenase model complex. In the gas phase, the energy barrier of the first transition state TS1 species is ca. 6.1 kcal/mol higher than the second transition state TS2 species. However, when the solvation effects were included, the energy order was reversed, i.e., the energy barrier of TS1 falls ca. 1.2 kcal/mol lower than TS2, indicating that the insertion of the second CO to iron is the rate-determining step in the whole transformation process. The initial insertion of the CO plays an important role in increasing the reaction barrier of the binding of a second CO, which prevented the second step transformation. Thus, the solvation effects play a significant role in determining the reaction mechanism. In addition, the energy of PC species is lower than RC species, demonstrating that this transformation is a significantly exothermic process. (C) 2015 Elsevier B.V. All rights reserved.
Language英语
WOS IDWOS:000356637200006
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/146330
Collection中国科学院大连化学物理研究所
Affiliation1.Henan Normal Univ, Coll Phys & Elect Engn, Xinxiang 453007, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Mol React Dynam, Dalian 116023, Peoples R China
3.Dalian Univ Technol, Sch Environm Sci & Technol, Key Lab Ind Ecol & Environm Engn MOE, Dalian 116024, Peoples R China
Recommended Citation
GB/T 7714
Li, Chaozheng,Fu, Zhiqiang,Zhang, Xiaoqian,et al. Theoretical study of iron acyl complexes modeling the active site of [Fe]-hydrogenase: Solvation effects play a significant role[J]. COMPUTATIONAL AND THEORETICAL CHEMISTRY,2015,1064:45-50.
APA Li, Chaozheng,Fu, Zhiqiang,Zhang, Xiaoqian,Liu, Yufang,&Wang, Yong.(2015).Theoretical study of iron acyl complexes modeling the active site of [Fe]-hydrogenase: Solvation effects play a significant role.COMPUTATIONAL AND THEORETICAL CHEMISTRY,1064,45-50.
MLA Li, Chaozheng,et al."Theoretical study of iron acyl complexes modeling the active site of [Fe]-hydrogenase: Solvation effects play a significant role".COMPUTATIONAL AND THEORETICAL CHEMISTRY 1064(2015):45-50.
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