How Accurate Can a Local Coupled Cluster Approach Be in Computing the Activation Energies of Late-Transition-Metal-Catalyzed Reactions with Au, Pt, and Ir?
文献类型：期刊论文
| 作者 | Kang, Runhua1; Lai, Wenzhen2; Yao, Jiannian1; Shaik, Sason3,4; Chen, Hui1 |
| 刊名 | JOURNAL OF CHEMICAL THEORY AND COMPUTATION
 |
| 出版日期 | 2012-09-01 |
| 卷号 | 8期号:9页码:3119-3127 |
| ISSN号 | 1549-9618 |
| DOI | 10.1021/ct3003942 |
| 英文摘要 | To improve the accuracy of local coupled cluster (LCC) methods in computing activation energies, we propose herein a new computational scheme. Its applications to various types of late-transition-metal-catalyzed reactions involving Au, Pt, and Ir indicate that the new corrective approach for LCC methods can downsize the mean unsigned deviation and maximum deviation, from the CCSD(T)/CBS reference, to about 0.3 and 0.9 kcal/mol. Using this method, we also calibrated the performance of popular density functionals, with respect to the same test set of reactions. It is concluded that the best functional is the general-purpose double hybrid functional B2GP-PLYP. Other well-performing functionals include the "kinetic" functionals M06-2X and BMK, which have a large percentage of HF exchange, and general-purpose functionals like PBE0 and wB97X. Comparatively, general-purpose functionals like PBE0 and TPSSh perform much better than the tested "kinetic" functionals for Pt-/Ir-catalyzed reactions, while the opposite is true for Au-catalyzed reactions. In contrast, wB97X performs more uniformly in these two classes of reactions. These findings hint that even within the scope of late transition metals, different types of reactions may require different types of optimal DFT methods. Empirical dispersion correction of DFT was found to have a small or no effect on the studied reactions barriers. |
| 语种 | 英语 |
| WOS记录号 | WOS:000308830700017 |
| 出版者 | AMER CHEMICAL SOC |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/48645]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | Yao, Jiannian |
| 作者单位 | 1.Chinese Acad Sci, BNLMS, Inst Chem, CAS Key Lab Photochem, Beijing 100190, Peoples R China 2.Renmin Univ China, Dept Chem, Beijing 100872, Peoples R China 3.Hebrew Univ Jerusalem, Inst Chem, IL-91904 Jerusalem, Israel 4.Hebrew Univ Jerusalem, Lise Meitner Minerva Ctr Computat Quantum Chem, IL-91904 Jerusalem, Israel |
| 推荐引用方式 GB/T 7714 | Kang, Runhua,Lai, Wenzhen,Yao, Jiannian,et al. How Accurate Can a Local Coupled Cluster Approach Be in Computing the Activation Energies of Late-Transition-Metal-Catalyzed Reactions with Au, Pt, and Ir?[J]. JOURNAL OF CHEMICAL THEORY AND COMPUTATION,2012,8(9):3119-3127. |
| APA | Kang, Runhua,Lai, Wenzhen,Yao, Jiannian,Shaik, Sason,&Chen, Hui.(2012).How Accurate Can a Local Coupled Cluster Approach Be in Computing the Activation Energies of Late-Transition-Metal-Catalyzed Reactions with Au, Pt, and Ir?.JOURNAL OF CHEMICAL THEORY AND COMPUTATION,8(9),3119-3127. |
| MLA | Kang, Runhua,et al."How Accurate Can a Local Coupled Cluster Approach Be in Computing the Activation Energies of Late-Transition-Metal-Catalyzed Reactions with Au, Pt, and Ir?".JOURNAL OF CHEMICAL THEORY AND COMPUTATION 8.9(2012):3119-3127. |
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来源：化学研究所
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