Dynamic Reconstruction of Ni/In2O3/ZrO2 Catalyst in Reverse Water‐Gas Conversion Reaction

The reconfiguration of catalysts in situ will obviously affect their catalytic performance, while the evolution process and the mechanism of reaction process remain unclear. Herein, a series of ternary Ni/In 2 O 3 /ZrO 2 catalysts is prepared by the two‐step method. In the reaction atmosphere (CO 2 /H 2 ), In 2 O 3 particles are highly dispersed on the carrier ZrO 2 , and are partially reduced to form InO x layers. Moreover, In 2 O 3 tends to migrate near Ni species, forming the NiInO x complex structure decorated by InO x layers. It is demonstrated that indium oxide serves as the main active site in the reverse water‐gas conversion reaction, and Ni species function as an auxiliary agent to generate the strong metal‐support interaction effect with indium oxide, facilitate the formation of the key intermediates HCOO* and CO*, and further enhance the CO yield. Ab initio molecular dynamics and density functional theory calculations confirm that the In 2 O 3 clusters have undergone dynamic structural reconstruction on the ZrO 2 support driven by temperature, and In 2 O 3 serves as the preferential adsorption site for CO 2 .