Efficient Liberation of Ammonia from Thermal Reaction of ScNH+ Cations and Water

Ming Wang, Chuan Xin Sun, Yue Zhao, Jia Tong Cui, Jia Bi Ma*

*此作品的通讯作者

科研成果: 期刊稿件文章同行评审

1 引用 (Scopus)

摘要

Ammonia synthesis by using water as a hydrogen source is a challenging task. Laser-ablation-generated ScNH+ cations have been mass-selected using a quadrupole mass filter and reacted with H2O in a linear ion trap reactor under thermal collision conditions. Through mass spectrometry in conjunction with density functional theory calculations, we found that ammonia is released as the product in the reaction of ScNH+ with H2O, and this reaction is with high efficiency and selectivity, and the rate constant for the reaction is (1.14 ± 0.23) × 10-10 cm3 molecule-1 s-1, corresponding to the reaction efficiency of 15%. Metal imido complexes (∗MNH) are one of the important intermediates in the currently reported NH3 synthetic reactions. The gas-phase ScNH+ cation can be a simplified model of∗MNH over catalysts of NH3 synthesis, and the facile proton transfer mechanism obtained in this model system may offer fundamental mechanistic insights into how to design catalysts for ammonia production by using water as the hydrogen source under ambient conditions.

源语言英语
页(从-至)7576-7581
页数6
期刊Journal of Physical Chemistry A
123
35
DOI
出版状态已出版 - 5 9月 2019

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Wang, M., Sun, C. X., Zhao, Y., Cui, J. T., & Ma, J. B. (2019). Efficient Liberation of Ammonia from Thermal Reaction of ScNH+ Cations and Water. Journal of Physical Chemistry A, 123(35), 7576-7581. https://doi.org/10.1021/acs.jpca.9b05890