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

Author

Listed:
  • 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
    University of Chinese Academy of Sciences)

  • Changbin Zhang

    (Chinese Academy of Sciences
    University of Chinese Academy of Sciences)

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.

Suggested Citation

  • Min Chen & Longgang Liu & Xueyan Chen & Xiaoxiao Qin & Jianghao Zhang & Shaohua Xie & Fudong Liu & Hong He & Changbin Zhang, 2024. "Sulfate residuals on Ru catalysts switch CO2 reduction from methanation to reverse water-gas shift reaction," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53909-8
    DOI: 10.1038/s41467-024-53909-8
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    2. Peng Yin & Xiao Luo & Yanfu Ma & Sheng-Qi Chu & Si Chen & Xusheng Zheng & Junling Lu & Xiao-Jun Wu & Hai-Wei Liang, 2021. "Sulfur stabilizing metal nanoclusters on carbon at high temperatures," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
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