Sulfate residuals on Ru catalysts switch CO2 reduction from methanation to reverse water-gas shift reaction

Min Chen, Longgang Liu, Xueyan Chen, Xiaoxiao Qin, Jianghao Zhang, Shaohua Xie, Fudong Liu (), Hong He and Changbin Zhang ()
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Min Chen: Chinese Academy of Sciences
Longgang Liu: Qufu Normal University
Xueyan Chen: Chinese Academy of Sciences
Xiaoxiao Qin: Chinese Academy of Sciences
Jianghao Zhang: Chinese Academy of Sciences
Shaohua Xie: University of California
Fudong Liu: University of California
Hong He: Chinese Academy of Sciences
Changbin Zhang: Chinese Academy of Sciences

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: Abstract Efficient heterogeneous catalyst design primarily focuses on engineering the active sites or supports, often neglecting the impact of trace impurities on catalytic performance. Herein, we demonstrate that even trace amounts of sulfate (SO42−) residuals on Ru/TiO2 can totally change the CO2 reduction from methanation to reverse-water gas shift (RWGS) reaction under atmospheric pressure. We reveal that air annealing causes the trace amount of SO42− to migrate from TiO2 to Ru/TiO2 interface, leading to the significant changes in product selectivity from CH4 to CO. Detailed characterizations and DFT calculations show that the sulfate at Ru/TiO2 interface notably enhances the H transfer from Ru particles to the TiO2 support, weakening the CO intermediate activation on Ru particles and inhibiting the further hydrogenation of CO to CH4. This discovery highlights the vital role of trace impurities in CO2 hydrogenation reaction, and also provides broad implications for the design and development of more efficient and selective heterogeneous catalysts.

Date: 2024
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DOI: 10.1038/s41467-024-53909-8

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