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Self-regeneration of supported transition metals by a high entropy-driven principle

Author

Listed:
  • Shengtai Hou

    (Shanghai Jiao Tong University)

  • Xuefeng Ma

    (Shanghai Jiao Tong University)

  • Yuan Shu

    (Shanghai Jiao Tong University)

  • Jiafeng Bao

    (Shanghai Jiao Tong University)

  • Qiuyue Zhang

    (Xiamen University)

  • Mingshu Chen

    (Xiamen University)

  • Pengfei Zhang

    (Shanghai Jiao Tong University)

  • Sheng Dai

    (Chemical Sciences Division, Oak Ridge National Laboratory)

Abstract

The sintering of Supported Transition Metal Catalysts (STMCs) is a core issue during high temperature catalysis. Perovskite oxides as host matrix for STMCs are proven to be sintering-resistance, leading to a family of self-regenerative materials. However, none other design principles for self-regenerative catalysts were put forward since 2002, which cannot satisfy diverse catalytic processes. Herein, inspired by the principle of high entropy-stabilized structure, a concept whether entropy driving force could promote the self-regeneration process is proposed. To verify it, a high entropy cubic Zr0.5(NiFeCuMnCo)0.5Ox is constructed as a host model, and interestingly in situ reversible exsolution-dissolution of supported metallic species are observed in multi redox cycles. Notably, in situ exsolved transition metals from high entropy Zr0.5(NiFeCuMnCo)0.5Ox support, whose entropic contribution (TΔSconfig = T⋆12.7 J mol−1 K−1) is predominant in ∆G, affording ultrahigh thermal stability in long-term CO2 hydrogenation (400 °C, >500 h). Current theory may inspire more STWCs with excellent sintering-resistance performance.

Suggested Citation

  • Shengtai Hou & Xuefeng Ma & Yuan Shu & Jiafeng Bao & Qiuyue Zhang & Mingshu Chen & Pengfei Zhang & Sheng Dai, 2021. "Self-regeneration of supported transition metals by a high entropy-driven principle," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26160-8
    DOI: 10.1038/s41467-021-26160-8
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    1. Simon A. Kondrat & Paul J. Smith & Peter P. Wells & Philip A. Chater & James H. Carter & David J. Morgan & Elisabetta M. Fiordaliso & Jakob B. Wagner & Thomas E. Davies & Li Lu & Jonathan K. Bartley &, 2016. "Stable amorphous georgeite as a precursor to a high-activity catalyst," Nature, Nature, vol. 531(7592), pages 83-87, March.
    2. Zhiqi Zhang & Yugang Chen & Liqi Zhou & Chi Chen & Zhen Han & Bingsen Zhang & Qiang Wu & Lijun Yang & Lingyu Du & Yongfeng Bu & Peng Wang & Xizhang Wang & Hui Yang & Zheng Hu, 2019. "The simplest construction of single-site catalysts by the synergism of micropore trapping and nitrogen anchoring," Nature Communications, Nature, vol. 10(1), pages 1-7, December.
    3. Y. Nishihata & J. Mizuki & T. Akao & H. Tanaka & M. Uenishi & M. Kimura & T. Okamoto & N. Hamada, 2002. "Self-regeneration of a Pd-perovskite catalyst for automotive emissions control," Nature, Nature, vol. 418(6894), pages 164-167, July.
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    1. Shuo Liu & Chaochao Dun & Qike Jiang & Zhengxi Xuan & Feipeng Yang & Jinghua Guo & Jeffrey J. Urban & Mark T. Swihart, 2024. "Challenging thermodynamics: combining immiscible elements in a single-phase nano-ceramic," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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