Accelerating Reverse Water Gas Shift Reaction through Synergistic CO<sub>2</sub> and H<sub>2</sub> Activation on Ru–Fe–(V<sub>O</sub>-in-CeO<sub>2</sub>) Ternary Catalytic Centers
Haoyang Jiang, Linyu Wang, Chuanhao Wang, Yi Xie, Caijuan Shi, Yongcheng Xiao, Yueren Liu, Weiping Ding, Miao Zhong
Abstract
The reverse water gas shift (RWGS) reaction shows promise for converting CO 2 emissions to chemical feedstocks using renewable H 2 . However, achieving high selectivity and activity at low temperatures remains challenging due to the thermodynamically more favorable CO 2 methanation reaction. Here we develop a robust Ru 0.0025 Ce 0.7 Fe 0.3 O 2−δ solid-solution nanorod catalyst featuring a ternary Fe–Ru–oxygen vacancy (V O ) center, overcoming limitations in intermediate adsorption and dissociation on single-component catalysts. Incorporating a trace amount of Ru (0.25 at. %) into Ce 0.7 Fe 0.3 O 2−δ markedly enhances CO 2 and H 2 dissociation and H 2 O formation, while the primary Ce 0.7 Fe 0.3 O 2−δ solid-solution component facilitates CO desorption, lowering the RWGS onset temperature to ∼200 °C. Experimental and computational analyses verify improved kinetics and stable performance with Ru 0.0025 Ce 0.7 Fe 0.3 O 2−δ, yielding a CO production rate of 326 mmol g cat –1 h –1, ∼100% selectivity, and a 21% yield, approaching the thermodynamic limit within a 5 min batch reaction at ∼450 °C surface temperature under 300 W xenon lamp illumination.