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Hydrogen activation enabled by the interfacial frustrated Lewis pairs on cobalt borate nanosheets

Author:
Zhang, Sai, Huang, Zheng-Qing, Chen, Xiao, Gan, Jie, Duan, Xuezhi, Yang, Bolun, Chang, Chun-Ran, Qu, Yongquan
Source:
Journal of catalysis 2019 v.372 pp. 142-150
ISSN:
0021-9517
Subject:
Fourier transform infrared spectroscopy, activation energy, active sites, borates, catalysts, catalytic activity, cobalt, dissociation, heterolytic cleavage, hydrogen, hydrogenation, isotopes, kinetics, moieties, nanosheets, physicochemical properties
Abstract:
Precisely controlling the surface physicochemical properties of a solid is critical to construct novel catalytic sites for various heterogeneous catalytic reactions. Herein, the interfacial frustrated Lewis pairs on cobalt borate (CoBOx) nanosheets are constructed by the surface hydroxyl on the top of one surface Co atom as the independent Lewis basic site and adjacent interfacial cobalt ion as the independent Lewis acidic site, enabling the efficient hydrogen activation as well as subsequent hydrogenation activity. Theoretical calculations and isotope experiments show that such a FLP site triggers the heterolytic hydrogen dissociation with a low activation energy of 0.37 eV. The catalytic performance, computational results, kinetic analysis and in-situ Fourier transform infrared spectroscopy profiles indicate the abundance of the surface hydroxyl on the top of the surface Co atom is the key for the construction of the interfacial FLP sites and subsequent hydrogen activation on those sites. Such a strategy provides a feasible approach to design the heterogenized FLP catalysts by controlling the interfacial physicochemical properties in term of the surface hydroxyl groups.
Agid:
6332715