1. Theoretical understanding on all-solid frustrated Lewis pair sites of C2N anchored by single metal atom.
- Author
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Zhu, Yijia, Jian, Changping, Xue, Ruifang, Zhang, Wei, Guo, Rou, Gao, Yijing, Chen, De-Li, Zhang, Fumin, Zhu, Weidong, and Wang, Fang-Fang
- Subjects
LEWIS pairs (Chemistry) ,HETEROGENEOUS catalysts ,ATOMS ,METALS ,LEWIS acids ,NITROGEN cycle ,OXYGEN reduction ,TRANSITION metals - Abstract
The design of all-solid heterogeneous catalysts with frustrated Lewis pairs (FLPs) has attracted much attention recently because of their appealing low dissociation energy for H
2 molecules due to which a promotion of hydrogenation reaction is expected. The sterically encumbered Lewis acid (metal site) and base (nitrogen site) in the cavity of single transition metal atom-doped M/C2 N sheets make them potential candidates for the design of catalysts with FLPs, while a comprehensive understanding of their intrinsic property and reactivity is still lacking. Calculations show that the complete dissociation of the H2 molecule into two H* states at the N sites requires two steps: heterolytic cleavage of the H2 molecule and the transfer of H* from the metal site to the N site, which are strongly related to the acidity of the metal site. Ni/C2 N and Pd/C2 N, which outperform the other eight transition metal atom (M) anchored M/C2 N candidates, possess low energy barriers for the complete dissociation of H2 molecules, with values of only 0.30 and 0.20 eV, respectively. Furthermore, both Ni/C2 N and Pd/C2 N catalysts can achieve semi-hydrogenation of C2 H2 into C2 H4 , with overall barriers of 0.81 and 0.75 eV, respectively, which are lower than those reported for many other catalysts. It is speculated that M/C2 N catalysts with intrinsic FLPs may also find applications in other important hydrogenation reactions. [ABSTRACT FROM AUTHOR]- Published
- 2022
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