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Designing water resistant high entropy oxide materials

Author

Listed:
  • Mengyuan Zhang

    (Ningxia University
    Shanghai Jiao Tong University)

  • Ying Gao

    (Shanghai Jiao Tong University)

  • Chengmin Xie

    (Shanghai Jiao Tong University)

  • Xiaolan Duan

    (Shanghai Jiao Tong University)

  • Xiaoyan Lu

    (Ningxia University)

  • Kongliang Luo

    (Ningxia University)

  • Jian Ye

    (Ningxia University)

  • Xiaopeng Wang

    (Ningxia University)

  • Xinhua Gao

    (Ningxia University)

  • Qiang Niu

    (Ltd.Ordos)

  • Pengfei Zhang

    (Ningxia University
    Shanghai Jiao Tong University)

  • Sheng Dai

    (Oak Ridge National Lab)

Abstract

The ubiquitous presence of moisture usually shows adverse effects on industrial catalysis. Herein, a concept of engineering entropy to design water-resistant oxide catalysts is proposed. The C3H6 oxidation by spinel ACr2O4 (A=Ni, Mg, Cu, Zn, Co) catalysts is selected as a model. Through DFT calculation, the adsorption energy of C3H6, the dissociation energy of molecular H2O on the oxide surface, and the formation energy of oxygen vacancy all suggest better performance induced by higher configurational entropy. Indeed, (Ni0.2Mg0.2Cu0.2Zn0.2Co0.2)Cr2O4 experimentally show excellent water resistance (>100 h) in C3H6 oxidation, while in sharp contrast binary oxides (e.g., NiCr2O4, CoCr2O4) are deactivated in 20 h. H2O-TPD, in-situ Raman, and in-situ FTIR all confirm the low H2O adsorption energy and strong hydrothermal stability of high entropy oxide, which is attributed to their lower Gibbs free energy. This work may inspire the rational design of water-resistant catalysts.

Suggested Citation

  • Mengyuan Zhang & Ying Gao & Chengmin Xie & Xiaolan Duan & Xiaoyan Lu & Kongliang Luo & Jian Ye & Xiaopeng Wang & Xinhua Gao & Qiang Niu & Pengfei Zhang & Sheng Dai, 2024. "Designing water resistant high entropy oxide materials," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-52531-y
    DOI: 10.1038/s41467-024-52531-y
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