As is well known, catalytic performance is close to interfacial properties of the catalysts, but the related properties of the interfaces are difficult to regulate precisely and simultaneously, including the metal states, acid-basic sites, defects and so on. In this work, the interfacial properties of In2O3 are controllable modified through different synthetic methods, in which the metastable of Inδ+ (2<δ<3) is mainly introduced by hydrothermal preparation, and oxygen vacancies (Ov) are produced due to heating induced phenomena in N2 calcination. At this situation, the massive formation of Inδ+ species further contribute to the formation of abundant oxygen vacancies and basic sites. More oxygen vacancies will lead to the strong adsorption of CO2 on the surface of In2O3, while the basic sites are benefit for the generation of formic acid intermediates during the reaction process. Therefore, the formation of abundant Inδ+-Ov interface in H-In2O3-N2 will facilitate to the CO2 dehydrogenation to methanol with high conversion and selectively, and the highest methanol spatiotemporal yield of 0.46 gCH3OH gcat-1 h-1 is obtained, which is 4.6 times higher than that of C-In2O3-N2 with less Inδ+-Ov interface. This method of controllable modification of Inδ+-Ov interface in In2O3 catalyst would also provide a valuable insight for other metal oxide catalysts in CO2 hydrogenation to methanol.

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