Reactivity of Tantalum Carbide Cluster Anions TaCn- (n=1-4) with Dinitrogen
文献类型：期刊论文
| 作者 | Mo, Li-Hui1,2; Liu, Qing-Yu1; Zhang, Ting1,2; Li, Zi-Yu1; He, Sheng-Gui1,2 |
| 刊名 | JOURNAL OF PHYSICAL CHEMISTRY A
 |
| 出版日期 | 2018-04-05 |
| 卷号 | 122期号:13页码:3489-3495 |
| ISSN号 | 1089-5639 |
| DOI | 10.1021/acs.jpca.8b01329 |
| 英文摘要 | Dinitrogen activation/fixation is one of the most important and challenging subjects in synthetic as well as theoretical chemistry. In this study, the adsorptioni reactions of N-2 onto TaCn- (n = 1-4) cluster anions have been investigated by means of mass spectrometry in conjunction with density functional theory calculations. Following the experimental results that only TaC4- was observed to adsorb N-2, theoretical calculations predicted that the TaC4- reaction system (TC4- + N2 -> TaC4N2-) has a negligible barrier on the approach of N-2 molecule while insurmountable barriers are located on the reaction pathways of TaC1-3-/N-2 reaction systems. The natural bond orbital and molecular orbital analysis indicated that the more positive charge on the metal center of TaC1-4- would facilitate the initial approach of the nonpolar N-2 molecule, and the appropriate frontier orbital of TaC1-4- with proper symmetry (pi-type Sd orbital) which can match up well with the pi* antibonding orbital of the N-2 molecule with less 6 repulsion and more possibility for Aback-donation would be helpful for the formation of the stable encounter complexes. This study reveals the fundamental rules and key factors governing the N-2 adsorption. |
| 语种 | 英语 |
| 出版者 | AMER CHEMICAL SOC |
| WOS记录号 | WOS:000429625900017 |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/46057]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | Li, Zi-Yu; He, Sheng-Gui |
| 作者单位 | 1.Chinese Acad Sci, CAS Res Educ Ctr Excellence Mol Sci, Inst Chem,Beijing Natl Lab Mol Sci, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China 2.Univ Chinese Acad Sci, Beijing 100049, Peoples R China |
| 推荐引用方式 GB/T 7714 | Mo, Li-Hui,Liu, Qing-Yu,Zhang, Ting,et al. Reactivity of Tantalum Carbide Cluster Anions TaCn- (n=1-4) with Dinitrogen[J]. JOURNAL OF PHYSICAL CHEMISTRY A,2018,122(13):3489-3495. |
| APA | Mo, Li-Hui,Liu, Qing-Yu,Zhang, Ting,Li, Zi-Yu,&He, Sheng-Gui.(2018).Reactivity of Tantalum Carbide Cluster Anions TaCn- (n=1-4) with Dinitrogen.JOURNAL OF PHYSICAL CHEMISTRY A,122(13),3489-3495. |
| MLA | Mo, Li-Hui,et al."Reactivity of Tantalum Carbide Cluster Anions TaCn- (n=1-4) with Dinitrogen".JOURNAL OF PHYSICAL CHEMISTRY A 122.13(2018):3489-3495. |
入库方式： OAI收割
来源：化学研究所
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