Photoelectron spectroscopy and formation mechanism of Ta2N3−: Activation of N2 by Ta2N−
Abstract
This work investigated the reaction mechanism of N2 on Ta2N− via the photoelectron spectroscopy study of Ta2N3−, focusing on the activation of nitrogen molecules (N2) by Ta2N−. The vertical detachment energy of Ta2N3− was determined to be 2.22 eV from the experimental photoelectron spectrum. Charge and bond order analyses reveal significant electron transfer from Ta to N and strong Ta–N bonding, supporting the relative stability and reactivity of the cluster. Energy decomposition analysis and natural orbitals for chemical valence analysis show that orbital interactions, especially π- and σ-donations from Ta2N− to N2, dominate the activation process of N2. Substantial charge transfer occurs from the Ta2N− fragment to the N2 fragment, accompanied by noticeable polarization, which facilitates the breaking of the N≡N bond. The results highlight the importance of Ta–N bond coordination in stabilizing dissociated nitrogen atoms, making Ta2N− a potentially efficient species for N2 activation.
Article Details
Journal Info
The Journal of Chemical Physics
American Institute of Physics
Authors (9)
Yong-Hang Zhang
College of Information Science and Engineering, Huaqiao University 1 , Xiamen 361021,
Peng Wang
Kai-Wen Liu
Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences 2 , Beijing 100190,
Huai-Qian Wang
College of Information Science and Engineering, Huaqiao University 1 , Xiamen 361021,
Hong-Guang Xu
Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences 2 , Beijing 100190,
Hui-Fang Li
Department of Infectious Diseases, State Key Laboratory of Virology and Biosafety, Frontier Science Center for Immunology and Metabolism, Medical Research Institute, Zhongnan Hospital of Wuhan University, Taikang Center for Life and Medical Sciences, Wuhan University
Jia-Ming Zhang
College of Information Science and Engineering, Huaqiao University 1 , Xiamen 361021,
Hao Zheng
Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, China
Wei-Jun Zheng
Beijing National Laboratory for Molecular Sciences, State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences 2 , Beijing 100190,