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Entropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports

Author

Listed:
  • Haidi Xu

    (Sichuan University
    Chemical Sciences Division, Oak Ridge National Laboratory
    University of Tennessee)

  • Zihao Zhang

    (Chemical Sciences Division, Oak Ridge National Laboratory
    University of Tennessee)

  • Jixing Liu

    (University of Tennessee)

  • Chi-Linh Do-Thanh

    (University of Tennessee)

  • Hao Chen

    (University of Tennessee)

  • Shuhao Xu

    (Sichuan University)

  • Qinjing Lin

    (Sichuan University)

  • Yi Jiao

    (Sichuan University)

  • Jianli Wang

    (Sichuan University)

  • Yun Wang

    (Sinocat Environmental Technology Co. Ltd.)

  • Yaoqiang Chen

    (Sichuan University
    Sichuan University)

  • Sheng Dai

    (Chemical Sciences Division, Oak Ridge National Laboratory
    University of Tennessee)

Abstract

Single-atom catalysts (SACs) have attracted considerable attention in the catalysis community. However, fabricating intrinsically stable SACs on traditional supports (N-doped carbon, metal oxides, etc.) remains a formidable challenge, especially under high-temperature conditions. Here, we report a novel entropy-driven strategy to stabilize Pd single-atom on the high-entropy fluorite oxides (CeZrHfTiLa)Ox (HEFO) as the support by a combination of mechanical milling with calcination at 900 °C. Characterization results reveal that single Pd atoms are incorporated into HEFO (Pd1@HEFO) sublattice by forming stable Pd–O–M bonds (M = Ce/Zr/La). Compared to the traditional support stabilized catalysts such as Pd@CeO2, Pd1@HEFO affords the improved reducibility of lattice oxygen and the existence of stable Pd–O–M species, thus exhibiting not only higher low-temperature CO oxidation activity but also outstanding resistance to thermal and hydrothermal degradation. This work therefore exemplifies the superiority of high-entropy materials for the preparation of SACs.

Suggested Citation

  • Haidi Xu & Zihao Zhang & Jixing Liu & Chi-Linh Do-Thanh & Hao Chen & Shuhao Xu & Qinjing Lin & Yi Jiao & Jianli Wang & Yun Wang & Yaoqiang Chen & Sheng Dai, 2020. "Entropy-stabilized single-atom Pd catalysts via high-entropy fluorite oxide supports," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:11:y:2020:i:1:d:10.1038_s41467-020-17738-9
    DOI: 10.1038/s41467-020-17738-9
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    Cited by:

    1. Yanzhi Wang & Hangjuan He & Hao Lv & Fengrui Jia & Ben Liu, 2024. "Two-dimensional single-crystalline mesoporous high-entropy oxide nanoplates for efficient electrochemical biomass upgrading," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    2. Lei Su & Huaixun Huyan & Abhishek Sarkar & Wenpei Gao & Xingxu Yan & Christopher Addiego & Robert Kruk & Horst Hahn & Xiaoqing Pan, 2022. "Direct observation of elemental fluctuation and oxygen octahedral distortion-dependent charge distribution in high entropy oxides," Nature Communications, Nature, vol. 13(1), pages 1-10, December.

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