Solid Solution Derived Cu Clusters on Partially Reduced CuCeO2 with Abundant Oxygen Vacancies Enable Efficient Reverse Water Gas Reaction

Chem Asian J. 2024 Dec 25:e202401485. doi: 10.1002/asia.202401485. Online ahead of print.

Abstract

The reverse water gas shift (RWGS) reaction provides a convenient approach to convert CO2 to CO, which facilitates to achieve the goals of carbon peaking and carbon neutrality. Herein, the Cu/CeO2 catalyst prepared by a co-precipitation method using a mixture of Na2CO3 and NaOH at pH of 10 (sample Cu/CeO2-10) achieved an intrinsic reaction rate of 428.4 mmol•gcat-1•h-1 with 100% CO selectivity at 400 °C and CO2/H2 ratio of 1:4, which is much higher than Cu/CeO2 prepared by impregnation and other methods. Various characterizations showed the highest fraction of CuCeO2 solid solution in the calcined Cu/CeO2-10, and formed highly dispersed Cu clusters (~2.5 nm) on partially reduced CuCeO2 solid solution with abundant of oxygen vacancies upon reduction. The Cu and oxygen vacancies facilitates the activation of H2 and CO2, respectively, resulting in lowered H2 and CO2 reaction orders. As a result, the synergy between the two components enhanced the overall RWGS activity with lowered activation energy. Moreover, the optimal catalyst is very stable in 24h stability test without detectable agglomeration of Cu clusters.

Keywords: CO2 reduction; Cu/CeO2 catalysts; oxygen vacancy; reverse water gas shit reaction; solid solution.