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Research Article

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

Qian Xu1,2,§Xingwang Cheng2,§Ningqiang Zhang1Yi Tu2Lihui Wu2Haibin Pan2Jun Hu2Honghe Ding2Junfa Zhu2( )Yadong Li1,3( )
Department of Chemistry, Tsinghua University, Beijing 100084, China
National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei 230029, China
College of Chemistry and Materials Science, Anhui Normal University, Wuhu 241002, China

§ Qian Xu and Xingwang Cheng contributed equally to this work.

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Graphical Abstract

Pd nanoparticles/CeO2 and Pd1/CeO2 model catalysts were prepared and the NO + CO adsorption/reaction on both model catalysts were explored in detail.

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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Nano Research
Pages 8882-8892
Cite this article:
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 Research, 2023, 16(7): 8882-8892. https://doi.org/10.1007/s12274-023-5585-2
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Received: 13 December 2022
Revised: 03 February 2023
Accepted: 16 February 2023
Published: 14 April 2023
© Tsinghua University Press 2023
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