^(15)N/^(14)N Isotopic Exchange in the Dissociative Adsorption of N_(2) on Tantalum Nitride Cluster Anions Ta_(3)N_(3)

作     者：Zi-Yu Li Li-Hui Mou Gui-Duo Jiang Qing-Yu Liu Sheng-Gui He 李子玉;牟丽慧;姜桂朵;刘清宇;何圣贵

作者机构：State Key Laboratory for Structural Chemistry of Unstable and Stable SpeciesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of SciencesBeijing 100049China Beijing National Laboratory for Molecular Sciences and CAS Research/Education Center of Excellence in Molecular SciencesBeijing 100190China 

基　　金：supported by the National Natural Science Foundation of China(No.21973101 and No.21833011) the Youth Innovation Promotion Association CAS(No.2020034) the K.C.Wong Education Foundation 

出 版 物：《Chinese Journal of Chemical Physics》 (化学物理学报（英文）)

年 卷 期：2022年第35卷第1期

页      码：77-85,I0062,I0063页

摘      要：Adsorption and activation of dinitrogen(N_(2)) is an indispensable process in nitrogen *** nitride species continue to attract attention as a promsing catalyst for ammonia ***,the detailed mechanisms at a molecular level between reactive nitride species and N_(2) remain unclear at elevated temperature,which is important to understand the temperature effect and narrow the gap between the gas phase system and condensed phase ***,the ^(15)N/^(14)N isotopic exchange in the reaction between tantalum nitride cluster anions Ta_(3)^(14)N_(3)^(-) and ^(15)N_(2) leading to the regeneration of ^(14)N_(2)/^(14)N^(15)N was observed at elevated temperature(393-593 K)using mass *** the aid of theoretical calculations,the exchange mechanism and the effect of temperature to promote the dissociation of N_(2) on Ta_(3)N_(3)^(-) were elucidated.A comparison experiment for Ta_(3)^(14)N_(4)^(-)/^(15)N_(2) couple indicated that only desorption of ^(15)N_(2) from Ta_(3)^(14)N_(4)^(15)N_(2)^(-) took place at elevated *** different exchange behavior can be well understood by the fact that nitrogen vacancy is a requisite for the dinitrogen activation over metal nitride *** study may shed light on understanding the role of nitrogen vacancy in nitride species for ammonia synthesis and provide clues in designing effective catalysts for nitrogen fixation.

主 题 词：Temperature effect Dinitrogen activation Transition metal nitrides Nitrogen vacancy Isotopic exchange 

学科分类：081702[081702] 081705[081705] 08[工学] 0817[工学-轻工类] 080502[080502] 0805[工学-能源动力学] 

核心收录：

D　O　I：10.1063/1674-0068/cjcp2112286

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