Chinese Journal of Catalysis ›› 2024, Vol. 60: 242-252.DOI: 10.1016/S1872-2067(24)60021-5

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Redox-driven surface generation of highly active Pd/PdO interface boosting low-temperature methane combustion

Yuanlong Tana,b, Yafeng Zhanga, Ya Gaoc,1, Jingyuan Mad, Han Zhaoa, Qingqing Gua, Yang Sua, Xiaoyan Xue, Aiqin Wanga,f, Bing Yanga,*(), Guo-Xu Zhangc,*(), Xiao Yan Liua,*(), Tao Zhanga,b   

  1. aCAS Key Laboratory of Science and Technology on Applied Catalysis, iChEM Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
    bUniversity of Chinese Academy of Sciences, Beijing 100049, China
    cMIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage, School of Chemistry and Chemical Engineering, Harbin Institute of Technology, Harbin 150001, Heilongjiang, China
    dShanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201204, China
    eDalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences Dalian 116023, Liaoning, China
    fState Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences Dalian 116023, Liaoning, China
  • Received:2024-01-11 Accepted:2024-03-22 Online:2024-05-18 Published:2024-05-20
  • Contact: E-mail: byang@dicp.ac.cn (B. Yang), zhanggx@hit.edu.cn(G. Zhang), xyliu2003@dicp.ac.cn (X. Liu).
  • About author:First author contact:1Contributed equally to this work.
  • Supported by:
    NSFC Center for Single-Atom Catalysis(22388102);DNL Cooperation Fund, CAS(DNL202002);Key Research Program of Frontier Sciences, CAS(ZDBS-LY-7012);National Natural Science Foundation of China(22102180);National Natural Science Foundation of China(22072151);Fundamental Research Funds for the Central Universities(20720220009);Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0540000);China Postdoctoral Science Foundation(2023M733452);Dalian Institute of Chemical Physics(DICP I202107);CAS Project for Young Scientists in Basic Research(YSBR-022);DICP.CAS-Cardiff Joint Research Units(121421ZYLH20230008)

Abstract:

The supported Pd catalyst has been a benchmark for methane elimination. However, the active structures have been long under debate. Here, by the aberration-corrected high angle annular dark field scanning transmission electron microscopy, operando X-ray absorption spectroscopy and quasi in situ X-ray photoelectron spectroscopy, we revealed the two-dimensional metallic Pd bumps on the PdO surface (litchi-like structure) generated by the redox atmosphere under the lean condition as a highly active structure of the Pd/Al2O3 catalyst. The substantially increased Pd/PdO interfaces boost the methane combustion activity higher than the similar catalysts reported previously, and remarkably enhance the reaction rate by 15.5 and 10.7 times that of pure PdO or metallic Pd counterpart under lean condition at 300 °C, respectively. Density-functional theory calculations confirm the synergistic C-C bond activation of methane on the Pd/PdO interfaces. Our work provides new insight into the traditional understanding of the chemical state and particle size effects of the industrial Pd catalysts for methane oxidation.

Key words: In situ characterization, Nanoparticles, Palladium, Methane combustion, Interface