Petroleum Science >2022,??lssue 1:??- DOI: https://doi.org/10.1016/j.petsci.2021.10.021
Charge effects on quinoline hydrodenitrogenation catalyzed by Ni–Mo–S active sites-A theoretical study by DFT calculation Open?Access
文章信息
作者：Si-Jia Ding, Shao-Zhong Peng, Zuo-Jie Yan, Ji-Feng Wang, Shu-Jiao Jiang, Zhan-Lin Yang,
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引用方式：Si-Jia Ding, Shao-Zhong Peng, Zuo-Jie Yan, Ji-Feng Wang, Shu-Jiao Jiang, Zhan-Lin Yang, Charge effects on quinoline hydrodenitrogenation catalyzed by Ni–Mo–S active sites-A theoretical study by DFT calculation, Petroleum Science, Volume 19, Issue 1, 2022, Pages 339-344, https://doi.org/10.1016/j.petsci.2021.10.021.
文章摘要
Abstract
The charge distribution on Ni–Mo–S active sites can affect hydrodenitrogenation (HDN) activity. In this study, a series of model Ni–Mo–S were developed with various charge distributions. For comparison, the charge distribution effects on quinoline HDN were studied. The results show that a lack of electrons and extra protons can both lower the orbital eigenvalue of the Ni–Mo–S, leading to stronger adsorption of nitrogen-containing compounds and inhibition of ammonia desorption. Electron deficiency will improve the generation of active hydrogen on the active sites but inhibit hydrogen transfer to the nitrogen compounds; extra protons can provide H+ to the nitrogen compounds, which will flexibly transfer between the nitrogen compound and active sites, thus improving the cleavage of the C–N bond.
The charge distribution on Ni–Mo–S active sites can affect hydrodenitrogenation (HDN) activity. In this study, a series of model Ni–Mo–S were developed with various charge distributions. For comparison, the charge distribution effects on quinoline HDN were studied. The results show that a lack of electrons and extra protons can both lower the orbital eigenvalue of the Ni–Mo–S, leading to stronger adsorption of nitrogen-containing compounds and inhibition of ammonia desorption. Electron deficiency will improve the generation of active hydrogen on the active sites but inhibit hydrogen transfer to the nitrogen compounds; extra protons can provide H+ to the nitrogen compounds, which will flexibly transfer between the nitrogen compound and active sites, thus improving the cleavage of the C–N bond.
关键词
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Charge distribution; Ni–Mo–S active Sites; Quinoline; Hydrodenitrogenation; Quantum chemistry calculation