DFT Methods to Study the Reaction Mechanism of Iridium-Catalyzed Hydrogenation of Olefins: Which Functional Should be Chosen?
文献类型：期刊论文
| 作者 | Sun, Yihua; Chen, Hui |
| 刊名 | CHEMPHYSCHEM
 |
| 出版日期 | 2016-01-04 |
| 卷号 | 17期号:1页码:119-127 |
| 关键词 | ab initio calculations density functional theory calculations homogeneous catalysis hydrogenation iridium |
| 英文摘要 | To enable the selection of more accurate computational methods for the future theoretical exploration of the reaction mechanism of Ir-catalyzed olefin hydrogenation, we compared high-level ab initio coupled cluster and DFT calculations with a simplified model of Pfaltz's Ir/P,N-type catalyst for all four previously proposed Ir-I/Ir-III and Ir-III/Ir-V mechanisms. Through the systematic assessment of the DFT performances, the DFT empirical dispersion correction (DFT-D3) is found to be indispensable for improving the accuracy of relative energies between the Ir-I/Ir-III and Ir-III/Ir-V mechanisms. After including the DFT-D3 correction, the three best performing density functionals (DFs) are B2-PLYP, BP86, and TPSSh. In these recommended DFs, the computationally more expensive double-hybrid functional B2-PLYP-D3 has a balanced and outstanding performance for calculations of the reaction barriers, reaction energies, and energy gaps between different mechanisms, whereas the less costly BP86-D3 and TPSSh-D3 methods have outstanding, but relatively less uniform performances. |
| 收录类别 | SCI |
| 语种 | 英语 |
| 公开日期 | 2016-05-09 |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/29746]  |
| 专题 | 化学研究所_光化学实验室 |
| 作者单位 | Chinese Acad Sci, Inst Chem, CAS Key Lab Photochem, BNLMS, Beijing 100190, Peoples R China |
| 推荐引用方式 GB/T 7714 | Sun, Yihua,Chen, Hui. DFT Methods to Study the Reaction Mechanism of Iridium-Catalyzed Hydrogenation of Olefins: Which Functional Should be Chosen?[J]. CHEMPHYSCHEM,2016,17(1):119-127. |
| APA | Sun, Yihua,&Chen, Hui.(2016).DFT Methods to Study the Reaction Mechanism of Iridium-Catalyzed Hydrogenation of Olefins: Which Functional Should be Chosen?.CHEMPHYSCHEM,17(1),119-127. |
| MLA | Sun, Yihua,et al."DFT Methods to Study the Reaction Mechanism of Iridium-Catalyzed Hydrogenation of Olefins: Which Functional Should be Chosen?".CHEMPHYSCHEM 17.1(2016):119-127. |
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来源：化学研究所
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