Dinitrogen Activation by Heteronuclear Metal Carbide Cluster Anions Y1-3CoC1,2: An Experimental and DFT Study

Meng Meng Wang, Ming Wang, Zhi Wen Ji, Xiao Meng Huang, Han Bin He, Xun Lei Ding*, Jia Bi Ma*

*此作品的通讯作者

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摘要

Mass spectrometry was used to observe the reactions between Y−Co heteronuclear metal carbide cluster anions Y1-3CoC1,2 and N2 at room temperature. Y2CoC1,2 can produce Co ejection products, in which Y2CoC also has N2 association products; YCoC2 and Y3CoC only generate N2 association products, while YCoC and Y3CoC2 are inert to N2. Detailed reaction pathways were obtained through density functional theory calculations, which reasonably explain the experimental phenomena. Co is superior to Y as the electrophilic reaction site in the clusters and is the preferential initial adsorption site for N2. Some crucial steps were identified, including N−N dissociation, CC−N formation, C−CN dissociation, and C−N formation. The energy barriers of these steps are closely related to the coordination mode of N/N2 and C/C2 in clusters. Two indicators, the N−N bond length and the Mayer bond order, were utilized to describe the activation degree of the N−N bond. Analyses on the density of states and the frontier molecular orbitals reveal the electronic structures of key intermediates for N−N dissociation. The reaction mechanisms of N2 activation on Y−Co carbide clusters obtained may lay a preliminary foundation for the further development of catalysts for nitrogen reduction reaction (NRR).

源语言英语
文章编号e202300978
期刊ChemCatChem
16
7
DOI
出版状态已出版 - 8 4月 2024

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Wang, M. M., Wang, M., Ji, Z. W., Huang, X. M., He, H. B., Ding, X. L., & Ma, J. B. (2024). Dinitrogen Activation by Heteronuclear Metal Carbide Cluster Anions Y1-3CoC1,2: An Experimental and DFT Study. ChemCatChem, 16(7), 文章 e202300978. https://doi.org/10.1002/cctc.202300978