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Integrating few-atom layer metal on high-entropy alloys to catalyze nitrate reduction in tandem

Author

Listed:
  • Jiace Hao

    (Jiangnan University)

  • Tongde Wang

    (Tongji University)

  • Ruohan Yu

    (Wuhan University of Technology)

  • Jian Cai

    (Jiangnan University)

  • Guohua Gao

    (Tongji University)

  • Zechao Zhuang

    (Tsinghua University
    Columbia University)

  • Qi Kang

    (Tongji University)

  • Shuanglong Lu

    (Jiangnan University)

  • Zhenhui Liu

    (Nanjing University of Aeronautics and Astronautics)

  • Jinsong Wu

    (Wuhan University of Technology)

  • Guangming Wu

    (Tongji University)

  • Mingliang Du

    (Jiangnan University)

  • Dingsheng Wang

    (Tsinghua University)

  • Han Zhu

    (Jiangnan University)

Abstract

While high-entropy alloy (HEA) catalysts seem to have the potential to break linear scaling relationships (LSRs) due to their structural complexity, the weighted averaging of properties among multiple principal components actually makes it challenging to diverge from the symmetry dependencies imposed by the LSRs. Herein, we develop a ‘surface entropy reduction’ method to induce the exsolution of a component with weak affinity for others, resulting in the formation of few-atom-layer metal (FL-M) on the surface of HEAs. These exsolved FL-M surpass the confines of the original configurational space of conventional HEAs, and collaborate with the HEA substrate, serving as geometrically separated active sites for multiple intermediates in a complex reaction. This FL-M-covered HEA shows an outstanding performance for electrocatalytic reduction of nitrate to ammonia (NH3) with a Faradaic efficiency of 92.7%, an NH3 yield rate of 2.45 mmol h–1 mgcat.–1, and high long-term stability (>200 h). Our work achieves the precise manipulation of atomic arrangement, thereby expanding both the chemical space occupied by known HEA catalysts and their potential application scenarios.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53427-7
    DOI: 10.1038/s41467-024-53427-7
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    References listed on IDEAS

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    1. Jia-Yi Fang & Qi-Zheng Zheng & Yao-Yin Lou & Kuang-Min Zhao & Sheng-Nan Hu & Guang Li & Ouardia Akdim & Xiao-Yang Huang & Shi-Gang Sun, 2022. "Ampere-level current density ammonia electrochemical synthesis using CuCo nanosheets simulating nitrite reductase bifunctional nature," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    2. 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.
    3. Chade Lv & Lixiang Zhong & Hengjie Liu & Zhiwei Fang & Chunshuang Yan & Mengxin Chen & Yi Kong & Carmen Lee & Daobin Liu & Shuzhou Li & Jiawei Liu & Li Song & Gang Chen & Qingyu Yan & Guihua Yu, 2021. "Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide," Nature Sustainability, Nature, vol. 4(10), pages 868-876, October.
    4. Gao-Feng Chen & Yifei Yuan & Haifeng Jiang & Shi-Yu Ren & Liang-Xin Ding & Lu Ma & Tianpin Wu & Jun Lu & Haihui Wang, 2020. "Electrochemical reduction of nitrate to ammonia via direct eight-electron transfer using a copper–molecular solid catalyst," Nature Energy, Nature, vol. 5(8), pages 605-613, August.
    5. Qingqing Ding & Yin Zhang & Xiao Chen & Xiaoqian Fu & Dengke Chen & Sijing Chen & Lin Gu & Fei Wei & Hongbin Bei & Yanfei Gao & Minru Wen & Jixue Li & Ze Zhang & Ting Zhu & Robert O. Ritchie & Qian Yu, 2019. "Tuning element distribution, structure and properties by composition in high-entropy alloys," Nature, Nature, vol. 574(7777), pages 223-227, October.
    6. 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.
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