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 |
| DOI | 10.1002/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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