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Unraveling the advantages of Pd/CeO2 single-atom catalysts in the NO + CO reaction by model catalysts

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Abstract

Selective catalytic reduction of NO by CO is challenging in environmental catalysis but attractive owing to the advantage of simultaneous elimination of NO and CO. Here, model catalysts consisting of Pd nanoparticles (NPs) and single-atom Pd supported on a CeO2 (111) film grown on Cu (111) (denoted as Pd NPs/CeO2 and Pd1/CeO2, respectively) were successfully prepared and characterized by synchrotron radiation photoemission spectroscopy (SRPES) and infrared reflection absorption spectroscopy (IRAS). The NO + CO adsorption/reaction on the Pd1/CeO2 and Pd NPs/CeO2 catalysts were carefully investigated using SRPES, temperature-programmed desorption (TPD), and IRAS. It is found that the reaction products on both model catalysts are in good agreement with those on real catalysts, demonstrating the good reliability of using these model catalysts to study the reaction mechanism of the NO + CO reaction. On the Pd NPs/CeO2 surface, N2 is formed by the combination of atomic N coming from the dissociation of NO on Pd NPs at higher temperatures. N2O formation occurs probably via chemisorbed NO combined with atomic N on the surface. While on the single-atom Pd1/CeO2 surface, no N2O is detected. The 100% N2 selectivity may stem from the formation of O-N-N-O* intermediate on the surface. Through this study, direct experimental evidence for the reaction mechanisms of the NO + CO reaction is provided, which supports the previous density functional theory (DFT) calculations.

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Acknowledgments

This work was financially supported by the National Natural Science Foundation of China (Nos. 21872131, 22106085, U1832218, and U1932214) and the National Key Research and Development Program of China (No. 2019YFA0405601).

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  1. Qian Xu and **ngwang Cheng contributed equally to this work.

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  1. Department of Chemistry, Tsinghua University, Bei**g, 100084, China

    Qian Xu, Ningqiang Zhang & Yadong Li

  2. National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, 230029, China

    Qian Xu, **ngwang Cheng, Yi Tu, Lihui Wu, Haibin Pan, Jun Hu, Honghe Ding & Junfa Zhu

  3. College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241002, China

    Yadong Li

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Xu, Q., Cheng, X., Zhang, N. et al. Unraveling the advantages of Pd/CeO2 single-atom catalysts in the NO + CO reaction by model catalysts. Nano Res. 16, 8882–8892 (2023). https://doi.org/10.1007/s12274-023-5585-2

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