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Identifying the roles of Ce3+−OH and Ce−H in the reverse water-gas shift reaction over highly active Ni-doped CeO2 catalyst

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Abstract

Nickel-CeO2-based materials are commonly used for the thermal catalytic hydrogenation of CO2. However, high Ni loadings and low CO selectivity restrict their use in the reverse water-gas shift (RWGS) reaction. Herein, we demonstrate a highly active, robust, and low-Ni-doped (1.1 wt.%) CeO2 catalyst (1.0−Ni−CeO2). The Ni-based-mass-specific CO formation rate reaches up to 1,542 mmol·gNi−1·h−1 with 100% CO selectivity at 300 °C for 100 h, among the best values reported in the literature. Density functional theory (DFT) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) results reveal that the enhanced catalytic activity is attributed to the abundant Ce−H species, while the high selectivity results from low CO affinity. More importantly, a new reaction mechanism is proposed, which involves the reduction of bicarbonate to generate formate intermediate and CO by the H− released from Ce−H species. The new findings in this work will benefit the design of economic, efficient, and robust catalysts for low-temperature RWGS reactions.

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Acknowledgements

This work was financially supported by the Science and Technology Project of Shenzhen (No. JCYJ20190806155814624), the National Natural Science Foundation of China (No. 22002120) and the Fundamental Research Funds for the Central Universities (No. 3102017jc01001). We would like to thank the Analytical & Testing Center of Northwestern Polytechnical University for SEM, TEM, XRD, and XPS characterizations.

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Authors and Affiliations

  1. Xi’an Key Laboratory of Functional Organic Porous Materials, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xi’an, 710129, China

    Haidong Shen, Yujuan Dong, Shaowei Yang, Yuan He, Qimeng Wang, Yueling Cao, Wenbin Wang, Tianshuai Wang, Qiuyu Zhang & Hepeng Zhang

  2. Research & Development Institute of Northwestern Polytechnical University in Shenzhen, Shenzhen, 518057, China

    Hepeng Zhang

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  1. Haidong Shen
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Correspondence to Tianshuai Wang, Qiuyu Zhang or Hepeng Zhang.

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Identifying the roles of Ce3+−OH and Ce−H in the reverse water-gas shift reaction over highly active Ni-doped CeO2 catalyst

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Shen, H., Dong, Y., Yang, S. et al. Identifying the roles of Ce3+−OH and Ce−H in the reverse water-gas shift reaction over highly active Ni-doped CeO2 catalyst. Nano Res. 15, 5831–5841 (2022). https://doi.org/10.1007/s12274-022-4207-8

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