With the development of industry, the emission of CO2 has caused a series of environmental problems. The utilization of CO2 has attracted a lot of attention in the chemical field. The catalytic reduction of CO2 to CO, known as the reverse water–gas shift (RWGS) reaction, was a potential pathway to utilize CO2, due to the product CO can be converted to high-value chemicals through the Fischer–Tropsch synthesis. However, the design of high-efficiency catalysts is still challenging. Due to the diversity of reactant molecules in the RWGS reaction, high-performance supported catalysts always require the cooperation of active metal and support. Herein, we present an active metal cluster-oxygen vacancy synergistic strategy, which achieves the construction of efficient supported catalysts. Firstly, the copper–ceria catalyst with stable copper clusters and abundant oxygen vacancies was constructed by introducing sufficient copper species (15 wt.%). Under harsh reaction conditions (600 °C, reductive atmosphere), the CeO2 nanorods suffered from partial sintering, but the copper species could be anchored on the partially sintered CeO2 in the form of highly dispersed clusters. Meanwhile, the copper clusters promoted the in-situ formation of high-density oxygen vacancies. The interface between copper cluster and oxygen vacancy facilitated the activation of CO2, thus promoted the RWGS reaction. Subsequently, we used the stress of MoO3/γ-Mo2N structure and the interaction between Pt and support to construct efficient catalyst with high-density Ptn-Ov synergistic sites. During the pretreatment process, surface MoO3 was transformed into MoOx with abundant oxygen vacancies, and isolated Pt atoms were converted to Pt clusters. By the combination of experiments and theoretical calculations, the synergistic interface between Pt clusters and oxygen vacancies was proved to be the active structure to promote the reaction.

Active metal cluster-oxygen vacancy synergistic strategy for the catalytic reduction of CO2 to CO

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