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  Dinitrogen Fixation and Reduction by Ta3N3H0,1- Cluster Anions at Room Temperature: Hydrogen-Assisted Enhancement of Reactivity

Zhao, Y., Cui, J.-T., Wang, M., Yubero Valdivielso, D., Fielicke, A., Hu, L.-R., et al. (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. doi:10.1021/jacs.9b03168.

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Datensatz-Permalink: https://hdl.handle.net/21.11116/0000-0004-9780-0 Versions-Permalink: https://hdl.handle.net/21.11116/0000-0006-CED9-E
Genre: Zeitschriftenartikel

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 Urheber:
Zhao, Yue1, Autor
Cui, Jia-Tong1, Autor
Wang, Ming1, Autor
Yubero Valdivielso, David2, 3, Autor           
Fielicke, André2, 3, Autor           
Hu, Lian-Rui4, Autor
Cheng, Xin5, Autor
Liu, Qing-Yu5, Autor
Li, Zi-Yu5, Autor
He, Sheng-Gui5, Autor
Ma, Jia-Bi1, Autor
Affiliations:
1Key Laboratory of Cluster Science of Ministry of Education, Beijing Key Laboratory of Photoelectronic/ElectrophotonicConversion Materials, School of Chemistry and Chemical Engineering, Beijing Institute of Technology, 100081 Beijing, China, ou_persistent22              
2Institute for Optics and Atomic Physics, Technische Universität Berlin, 10623 Berlin, Germany, ou_persistent22              
3Molecular Physics, Fritz Haber Institute, Max Planck Society, ou_634545              
4School of Science, Xihua University, 610039 Chengdu, China, ou_persistent22              
5State Key Laboratory for Structural Chemistry of Unstable and Stable Species, Institute of Chemistry, Chinese Academy ofSciences, 100190 Beijing, China, ou_persistent22              

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 Zusammenfassung: Dinitrogen activation and reduction is one of the mostchallenging and important subjects in chemistry. Herein, we report the N2 binding and reduction at the well-defined Ta3N3H- and Ta3N3- gas-phaseclusters by using mass spectrometry (MS), anion photoelectron spectros-copy (PES), and quantum-chemical calculations. The PES and calculationresults show clear evidence that N2 can be adsorbed and completelyactivated 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 N2 activation reactions mediated by Ta3N3H- and Ta3N3-; two and three Ta atoms are active sites and also electron donors for the N2 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 N2 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 N2 reduction, which provides molecular-level insights into the rational design of tantalum nitride-based catalysts for N2 fixation and activation or N3 synthesis.

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Sprache(n): eng - English
 Datum: 2019-03-282019-07-172019-08-14
 Publikationsstatus: Erschienen
 Seiten: 9
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/jacs.9b03168
 Art des Abschluß: -

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Titel: Journal of the American Chemical Society
  Alternativer Titel : J. Am. Chem. Soc.
  Alternativer Titel : JACS
Genre der Quelle: Zeitschrift
 Urheber:
Affiliations:
Ort, Verlag, Ausgabe: Washington, DC : American Chemical Society
Seiten: - Band / Heft: 141 (32) Artikelnummer: - Start- / Endseite: 12592 - 12600 Identifikator: n.a.: /journals/resource/954925376870