Geometric and electronic effects on the performance of a bifunctional Ru2P catalyst in the hydrogenation and acceptorless dehydrogenation of N-heteroarenes
Geometric and electronic effects on the performance of a bifunctional Ru2P catalyst in the hydrogenation and acceptorless dehydrogenation of N-heteroarenes
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DOI：
10.1016/s1872-2067(20)63747-0
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发表时间：
2021-07
影响因子：
16.5
通讯作者：
Fan Shao;Zihao Yao;Yijing Gao;Qiang Zhou;Zhikang Bao;G. Zhuang;Xing Zhong;Chuan Wu;Zhongzhe Wei-Z
中科院分区：
文献类型：
--
作者：
Fan Shao;Zihao Yao;Yijing Gao;Qiang Zhou;Zhikang Bao;G. Zhuang;Xing Zhong;Chuan Wu;Zhongzhe Wei-Z
开发用于N-杂环高效加氢和无受体脱氢的双功能催化剂是一个挑战。在这项研究中，Ru 2 P/AC有效地促进了不饱和和饱和N-杂环之间的可逆转化，产率分别为98%和99%。此外，一个显着的增强Ru 2 P/AC的重复使用性进行了观察相比，其他钌基催化剂。根据密度泛函理论计算，Ru 2 P/AC的上级性能归因于特定的协同因素，即P诱导的几何效应和电子效应。P极大地减少了Ru-Ru系综，精细地修饰了电子结构，导致催化剂的低反应势垒和高脱附能力，进一步促进了加氢和无受体脱氢过程。
The development of bifunctional catalysts for the efficient hydrogenation and acceptorless dehydrogenation ofN-heterocycles is a challenge. In this study, Ru2P/AC effectively promoted reversible transformations between unsaturated and saturatedN-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.