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Ru-based catalysts for efficient CO2 methanation: Synergistic catalysis between oxygen vacancies and basic sites

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Abstract

The fundamental insights of the reaction mechanism, especially the synergistic effect between oxygen vacancies and basic sites, are highly promising yet challenging for Ru-based catalysts during carbon dioxide (CO2) methanation. Herein, a series of Ru-based catalysts were employed to study the mechanism of CO2 methanation. It is found that Ru/CeO2 catalyst exhibits a much higher CO2 conversion (86%) and CH4 selectivity (100%), as well as excellent stability of 30 h due to the existence of abundant oxygen vacancies and weak basic sites. Additionally, the in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) and density functional theory (DFT) calculations reveal that the formate formation step dominated the hydrogenation route on Ru/CeO2 catalyst, and the b-HCOO* could be the key intermediate due to b-HCOO* is more easily hydrogenated to methane than m-HCOO*. The systematic study marks the significance of precise tailoring of the synergistic relationship between oxygen vacancies and basic sites for achieving the desired performance in CO2 methanation.

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Acknowledgements

This project has received funding from the National Natural Science Foundation of China (No. 22102215) and the Fundamental Research Funds for the Central Universities (Nos. 21CX06013A and 22CX03001A). This work was financially supported by the State Key Laboratory of Heavy Oil Processing and the Key Project of China National Key R&D Plan (No. 2018YFE0118200).

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  1. Chunfen Wang and Yonglian Lu contributed equally to this work.

Authors and Affiliations

  1. State Key Laboratory of Heavy Oil Processing, College of Chemistry and Chemical Engineering, China University of Petroleum (East China), Qingdao, 266580, China

    Chunfen Wang, Yonglian Lu, Yu Zhang, Hui Fu, Feng Li, Zhen Liu, Youhe Wang, Hongman Sun & Zifeng Yan

  2. School of Chemistry and Chemical Engineering, Queen’s University Belfast, Belfast, BT7 1NN, UK

    Shuzhuang Sun & Chunfei Wu

  3. State Key Laboratory of Solidification Processing, School of Materials Science and Engineering, Northwestern Polytechnical University, Xi’an, 710072, China

    Zhiyao Duan

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  1. Chunfen Wang
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Wang, C., Lu, Y., Zhang, Y. et al. Ru-based catalysts for efficient CO2 methanation: Synergistic catalysis between oxygen vacancies and basic sites. Nano Res. 16, 12153–12164 (2023). https://doi.org/10.1007/s12274-023-5592-3

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