ICCAS OpenIR
Dinitrogen Fixation and Reduction by Ta3N3H0,1- Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity
Zhao, Yue; Cui, Jia-Tong; Wang, Ming; Valdivielso, David Yubero; Fielicke, Andre; Hu, Lian-Rui; Cheng, Xin; Liu, Qjng-Yu; Li, Zi-Yu; He, Sheng-Gui; Ma, Jia-Bi
2019-08-14
Source PublicationJOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN0002-7863
Volume141Issue:32Pages:12592-12600
AbstractDinitrogen activation and reduction is one of the most challenging and important subjects in chemistry. Herein, we report the N-2 binding and reduction at the well-defined Ta3N3H- and Ta3N3- gas-phase clusters by using mass spectrometry (MS), anion photoelectron spectroscopy (PES), and quantum-chemical calculations. The PES and calculation results show clear evidence that N-2 can be adsorbed and completely activated by Ta3N3H- and Ta3N3- clusters, yielding to the products Ta3N5H- and Ta3N5-, but the reactivity of Ta3N3H- is five times higher than that of the dehydrogenated Ta3N3- clusters. The detailed mechanistic investigations further indicate that a dissociative mechanism dominates the N-2 activation reactions mediated by Ta3N3H- and Ta3N3-; two and three Ta atoms are active sites and also electron donors for the N-2 reduction, respectively. Although the hydrogen atom in Ta3N3H- is not directly involved in the reaction, its very presence modifies the charge distribution and the geometry of Ta3N3H-, which is crucial to increase the reactivity. The mechanisms revealed in this gas-phase study stress the fundamental rules for N-2 activation and the important role of transition metals as active sites as well as the new significant role of metal hydride bonds in the process of N-2 reduction, which provides molecular-level insights into the rational design of tantalum nitride-based catalysts for N-2 fixation and activation or NH3 synthesis.
DOI10.1021/jacs.9b03168
Indexed BySCI
Language英语
WOS IDWOS:000481563500026
EI Accession Number1520-5126
Citation statistics
Cited Times:2[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.iccas.ac.cn/handle/121111/82663
Collection中国科学院化学研究所
AffiliationChinese Acad Sci, Inst Chem, Beijing 100190, Peoples R China
Recommended Citation
GB/T 7714
Zhao, Yue,Cui, Jia-Tong,Wang, Ming,et al. Dinitrogen Fixation and Reduction by Ta3N3H0,1- Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2019,141(32):12592-12600.
APA Zhao, Yue.,Cui, Jia-Tong.,Wang, Ming.,Valdivielso, David Yubero.,Fielicke, Andre.,...&Ma, Jia-Bi.(2019).Dinitrogen Fixation and Reduction by Ta3N3H0,1- Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,141(32),12592-12600.
MLA Zhao, Yue,et al."Dinitrogen Fixation and Reduction by Ta3N3H0,1- Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 141.32(2019):12592-12600.
Files in This Item:
There are no files associated with this item.
Related Services
Recommend this item
Bookmark
Usage statistics
Export to Endnote
Google Scholar
Similar articles in Google Scholar
[Zhao, Yue]'s Articles
[Cui, Jia-Tong]'s Articles
[Wang, Ming]'s Articles
Baidu academic
Similar articles in Baidu academic
[Zhao, Yue]'s Articles
[Cui, Jia-Tong]'s Articles
[Wang, Ming]'s Articles
Bing Scholar
Similar articles in Bing Scholar
[Zhao, Yue]'s Articles
[Cui, Jia-Tong]'s Articles
[Wang, Ming]'s Articles
Terms of Use
No data!
Social Bookmark/Share
All comments (0)
No comment.
 

Items in the repository are protected by copyright, with all rights reserved, unless otherwise indicated.