中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
Hydrogenation of Carbon Dioxide to Methanol Catalyzed by Iron, Cobalt, and Manganese Cyclopentadienone Complexes: Mechanistic Insights and Computational Design

文献类型:期刊论文

作者Ge, Hongyu1,2; Chen, Xiangyang1,2; Yang, Xinzheng1
刊名CHEMISTRY-A EUROPEAN JOURNAL
出版日期2017-07-03
卷号23期号:37页码:8850-8856
关键词Base Metal Catalysts Computational Chemistry Cyclopentadienone Complexes Density Functional Calculations Hydrogenation
ISSN号0947-6539
DOI10.1002/chem.201701200
英文摘要Density functional theory study of the hydrogenation of carbon dioxide to methanol catalyzed by iron, cobalt, and manganese cyclopentadienone complexes reveals a self-promoted mechanism, which features a methanol-or water-molecule- assisted proton transfer for the cleavage of H-2. The total free energy barrier of the formation of methanol from CO2 and H-2 catalyzed by Knolker's iron cyclopentadienone complex, [2,5-(SiMe3)(2)- 3,4-(CH2)(4)(eta(5)-C4COH)] Fe( CO)(2)H, is 26.0 kcalmol(-1) in the methanol solvent. We also evaluated the catalytic activities of 8 other experimentally reported iron cyclopentadienone complexes and 37 iron, cobalt, and manganese cyclopentadienone complexes proposed in this study. In general, iron and manganese complexes have relatively higher catalytic activities. Among all calculated complexes, [2,5-(SiMe3)(2)-3,4-CH3CHSCH2(eta(5)-C4COH)] Fe(CO)(2)H (1(Fe-Casey-S-CH3)) is the most active one with a total free energy barrier of 25.1 kcalmol(-1) in the methanol solvent. Such a low barrier indicates that 1(Fe-Casey-S-CH3) is a very promising low-cost and high efficiency catalyst for the conversion of CO2 and H-2 to methanol under mild conditions.
语种英语
WOS记录号WOS:000404550000012
出版者WILEY-V C H VERLAG GMBH
源URL[http://ir.iccas.ac.cn/handle/121111/44963]  
专题中国科学院化学研究所
通讯作者Yang, Xinzheng
作者单位1.Chinese Acad Sci, Beijing Natl Lab Mol Sci, State Key Lab Struct Chem Unstable & Stable Speci, CAS Res Educ Ctr Excellence Mol Sci,Inst Chem, Beijing 100190, Peoples R China
2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China
推荐引用方式
GB/T 7714
Ge, Hongyu,Chen, Xiangyang,Yang, Xinzheng. Hydrogenation of Carbon Dioxide to Methanol Catalyzed by Iron, Cobalt, and Manganese Cyclopentadienone Complexes: Mechanistic Insights and Computational Design[J]. CHEMISTRY-A EUROPEAN JOURNAL,2017,23(37):8850-8856.
APA Ge, Hongyu,Chen, Xiangyang,&Yang, Xinzheng.(2017).Hydrogenation of Carbon Dioxide to Methanol Catalyzed by Iron, Cobalt, and Manganese Cyclopentadienone Complexes: Mechanistic Insights and Computational Design.CHEMISTRY-A EUROPEAN JOURNAL,23(37),8850-8856.
MLA Ge, Hongyu,et al."Hydrogenation of Carbon Dioxide to Methanol Catalyzed by Iron, Cobalt, and Manganese Cyclopentadienone Complexes: Mechanistic Insights and Computational Design".CHEMISTRY-A EUROPEAN JOURNAL 23.37(2017):8850-8856.

入库方式: OAI收割

来源:化学研究所

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