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Unraveling the electronegativity-dominated intermediate adsorption on high-entropy alloy electrocatalysts

Author

Listed:
  • Jiace Hao

    (Jiangnan University)

  • Zechao Zhuang

    (Tsinghua University)

  • Kecheng Cao

    (ShanghaiTech University)

  • Guohua Gao

    (Tongji University)

  • Chan Wang

    (Jiangnan University)

  • Feili Lai

    (KU Leuven)

  • Shuanglong Lu

    (Jiangnan University)

  • Piming Ma

    (Jiangnan University)

  • Weifu Dong

    (Jiangnan University)

  • Tianxi Liu

    (Jiangnan University)

  • Mingliang Du

    (Jiangnan University)

  • Han Zhu

    (Jiangnan University)

Abstract

High-entropy alloys have received considerable attention in the field of catalysis due to their exceptional properties. However, few studies hitherto focus on the origin of their outstanding performance and the accurate identification of active centers. Herein, we report a conceptual and experimental approach to overcome the limitations of single-element catalysts by designing a FeCoNiXRu (X: Cu, Cr, and Mn) High-entropy alloys system with various active sites that have different adsorption capacities for multiple intermediates. The electronegativity differences between mixed elements in HEA induce significant charge redistribution and create highly active Co and Ru sites with optimized energy barriers for simultaneously stabilizing OH* and H* intermediates, which greatly enhances the efficiency of water dissociation in alkaline conditions. This work provides an in-depth understanding of the interactions between specific active sites and intermediates, which opens up a fascinating direction for breaking scaling relation issues for multistep reactions.

Suggested Citation

  • Jiace Hao & Zechao Zhuang & Kecheng Cao & Guohua Gao & Chan Wang & Feili Lai & Shuanglong Lu & Piming Ma & Weifu Dong & Tianxi Liu & Mingliang Du & Han Zhu, 2022. "Unraveling the electronegativity-dominated intermediate adsorption on high-entropy alloy electrocatalysts," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-30379-4
    DOI: 10.1038/s41467-022-30379-4
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    References listed on IDEAS

    as
    1. Matthew W. Glasscott & Andrew D. Pendergast & Sondrica Goines & Anthony R. Bishop & Andy T. Hoang & Christophe Renault & Jeffrey E. Dick, 2019. "Electrosynthesis of high-entropy metallic glass nanoparticles for designer, multi-functional electrocatalysis," Nature Communications, Nature, vol. 10(1), pages 1-8, December.
    2. Kohsuke Mori & Naoki Hashimoto & Naoto Kamiuchi & Hideto Yoshida & Hisayoshi Kobayashi & Hiromi Yamashita, 2021. "Hydrogen spillover-driven synthesis of high-entropy alloy nanoparticles as a robust catalyst for CO2 hydrogenation," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
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    Cited by:

    1. Lin He & Menggang Li & Longyu Qiu & Shuo Geng & Yequn Liu & Fenyang Tian & Mingchuan Luo & Hu Liu & Yongsheng Yu & Weiwei Yang & Shaojun Guo, 2024. "Single-atom Mo-tailored high-entropy-alloy ultrathin nanosheets with intrinsic tensile strain enhance electrocatalysis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    2. Jiace Hao & Tongde Wang & Ruohan Yu & Jian Cai & Guohua Gao & Zechao Zhuang & Qi Kang & Shuanglong Lu & Zhenhui Liu & Jinsong Wu & Guangming Wu & Mingliang Du & Dingsheng Wang & Han Zhu, 2024. "Integrating few-atom layer metal on high-entropy alloys to catalyze nitrate reduction in tandem," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    3. Yuanfeng Li & Tian Qin & Yuechang Wei & Jing Xiong & Peng Zhang & Kezhen Lai & Hongjie Chi & Xi Liu & Liwei Chen & Xiaolin Yu & Zhen Zhao & Lina Li & Jian Liu, 2023. "A single site ruthenium catalyst for robust soot oxidation without platinum or palladium," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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