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Performance, Structure and Mechanisms of Pd Catalyst Supported on M-Doped (M = La, Ba and K) CeO2 for Methane Oxidation

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Abstract

In this study, the experiments were carried out to investigate the influence of Pd catalyst supported on M-doped (M = La, Ba and K) CeO2 for methane oxidation activity with a fixed-bed reactor. The structure, morphology and active species of Pd-M/CeO2 catalysts were thoroughly investigated with the means of TEM, BET, XRD, XPS, CO chemisorption, H2-TPR and CO2-TPD. The results showed that the catalytic activity order was Pd-La/CeO2 > Pd-Ba/CeO2 > Pd/CeO2 > Pd-K/CeO2. It was easier for more weak basic sites and PdOx clusters or particles to emerge on Pd-La/CeO2 catalyst surface and exhibited better redox performance. Ce3+/Ce4+ ions could be substituted by Ba2+ and accompanied with an increase in adsorbed oxygen on Pd-Ba/CeO2 catalyst surface. For Pd-K/CeO2 catalyst, the Pd dispersion was increased, but CeO2 appeared sintering in the calcination process. The in situ DRIFTs studies confirmed that the methane oxidation process over Pd-M/CeO2 catalysts was similar, which formed formic acid species and bidentate carbonate that transformed by monodentate. Furthermore, according to the generation of gaseous adsorption O2– ion at a specific temperature, it could be concluded that the oxidation process of methane on the Pd-La/CeO2 and Pd-Ba/CeO2 catalysts followed Mars-van Krevelen (MvK) and Eley–Rideal (E–R) mechanism, while Pd-K/CeO2 catalyst only existed MvK mechanism.

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Acknowledgements

Financial support of this paper was provided by the National Natural Science Foundation of China (Grant No. 51906089), Provincial Engineering Research Center for New Energy Vehicle Intelligent Control and Simulation Test Technology of Sichuan (Grant No. XNYQ2021-002), Zhenjiang City Key R&D Program (Grant No. GY2020016).

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Authors and Affiliations

  1. School of Automotive and Traffic Engineering, Jiangsu University, Zhenjiang, 212013, China

    Feixiang Li, Lili Lei, Jing Yi, Chenglong Dou & Pan Wang

  2. School of Automobile and Transportation, Xihua University, Chengdu, 610039, China

    Zhongwei Meng

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FL: Methodology, Writing—original draft. Lili Lei: Supervision. JY: Visualization, Investigation. CD: Visualization. ZM: Funding acquisition. PW: Data curation.

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Correspondence to Lili Lei.

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Li, F., Lei, L., Yi, J. et al. Performance, Structure and Mechanisms of Pd Catalyst Supported on M-Doped (M = La, Ba and K) CeO2 for Methane Oxidation. Catal Lett 153, 1847–1858 (2023). https://doi.org/10.1007/s10562-022-04124-x

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