Geometric and electronic effects on the performance of a bifunctional Ru2P catalyst in the hydrogenation and acceptorless dehydrogenation of N-heteroarenes

The development of bifunctional catalysts for the efficient hydrogenation and acceptorless dehydrogenation of N-heterocycles is a challenge. In this study, Ru2P/AC effectively promoted reversible transformations between unsaturated and saturated N-heterocycles affording yields of 98% and 99%, respec...

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Bibliographic Details
Published in:Chinese journal of catalysis Vol. 42; no. 7; pp. 1185 - 1194
Main Authors: Shao, Fangjun, Yao, Zihao, Gao, Yijing, Zhou, Qiang, Bao, Zhikang, Zhuang, Guilin, Zhong, Xing, Wu, Chuan, Wei, Zhongzhe, Wang, Jianguo
Format: Journal Article
Language:English
Published: Elsevier B.V 01.07.2021
Subjects:
Acceptorless dehydrogenation
Bifunction catalyst
Geometric and electronic effects
Hydrogenation
Reaction mechanism
Ruthenium phosphide
Acceptorless dehydrogenation
Reaction mechanism
Ruthenium phosphide
Bifunction catalyst
Geometric and electronic effects
Hydrogenation
ISSN:1872-2067, 1872-2067
Online Access:Get full text
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Summary:The development of bifunctional catalysts for the efficient hydrogenation and acceptorless dehydrogenation of N-heterocycles is a challenge. In this study, Ru2P/AC effectively promoted reversible transformations between unsaturated and saturated N-heterocycles affording yields of 98% and 99%, respectively. Moreover, a remarkable enhancement in the reusability of Ru2P/AC was observed compared with other Ru-based catalysts. According to density functional theory calculations, the superior performance of Ru2P/AC was ascribed to specific synergistic factors, namely geometric and electronic effects induced by P. P greatly reduced the large Ru-Ru ensembles and finely modified the electronic structures, leading to a low reaction barrier and high desorption ability of the catalyst, further boosting the hydrogenation and acceptorless dehydrogenation processes. The P element is the decisive factor! Ru2P/AC allowed for efficient reversible transformations between unsaturated and saturated N-heterocycles. The P atom finely modified the geometric and electronic structures, leading to a balance between reaction and diffusion, and boosting the hydrogenation and dehydrogenation processes.
ISSN:1872-2067
1872-2067
DOI:10.1016/S1872-2067(20)63747-0