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.

Jiang, Haoyang; Wang, Linyu; Wang, Chuanhao; Xie, Yi; Shi, Caijuan; Xiao, Yongcheng; Liu, Yueren; Ding, Weiping et al. · Nano Lett · 2025

basic_science · Level V

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Abstract

The reverse water gas shift (RWGS) reaction shows promise for converting CO<sub>2</sub> emissions to chemical feedstocks using renewable H<sub>2</sub>. However, achieving high selectivity and activity at low temperatures remains challenging due to the thermodynamically more favorable CO<sub>2</sub> methanation reaction. Here we develop a robust Ru<sub>0.0025</sub>Ce<sub>0.7</sub>Fe<sub>0.3</sub>O<sub>2-δ</sub> solid-solution nanorod catalyst featuring a ternary Fe-Ru-oxygen vacancy (V<sub>O</sub>) center, overcoming limitations in intermediate adsorption and dissociation on single-component catalysts. Incorporating a trace amount of Ru (0.25 at. %) into Ce<sub>0.7</sub>Fe<sub>0.3</sub>O<sub>2-δ</sub> markedly enhances CO<sub>2</sub> and H<sub>2</sub> dissociation and H<sub>2</sub>O formation, while the primary Ce<sub>0.7</sub>Fe<sub>0.3</sub>O<sub>2-δ</sub> 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<sub>0.0025</sub>Ce<sub>0.7</sub>Fe<sub>0.3</sub>O<sub>2-δ</sub>, yielding a CO production rate of 326 mmol g<sub>cat</sub><sup>-1</sup> h<sup>-1</sup>, ∼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.