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General synthesis of high-entropy single-atom nanocages for electrosynthesis of ammonia from nitrate

Author

Listed:
  • Sishuang Tang

    (The University of Texas at Austin)

  • Minghao Xie

    (The University of Texas at Austin)

  • Saerom Yu

    (The University of Texas at Austin)

  • Xun Zhan

    (The University of Texas at Austin)

  • Ruilin Wei

    (Fudan University)

  • Maoyu Wang

    (Argonne National Laboratory)

  • Weixin Guan

    (The University of Texas at Austin)

  • Bowen Zhang

    (The University of Texas at Austin)

  • Yuyang Wang

    (The University of Texas at Austin)

  • Hua Zhou

    (Argonne National Laboratory)

  • Gengfeng Zheng

    (Fudan University)

  • Yuanyue Liu

    (The University of Texas at Austin)

  • Jamie H. Warner

    (The University of Texas at Austin)

  • Guihua Yu

    (The University of Texas at Austin)

Abstract

Given the growing emphasis on energy efficiency, environmental sustainability, and agricultural demand, there’s a pressing need for decentralized and scalable ammonia production. Converting nitrate ions electrochemically, which are commonly found in industrial wastewater and polluted groundwater, into ammonia offers a viable approach for both wastewater treatment and ammonia production yet limited by low producibility and scalability. Here we report a versatile and scalable solution-phase synthesis of high-entropy single-atom nanocages (HESA NCs) in which Fe and other five metals-Co, Cu, Zn, Cd, and In-are isolated via cyano-bridges and coordinated with C and N, respectively. Incorporating and isolating the five metals into the matrix of Fe resulted in Fe-C5 active sites with a minimized symmetry of lattice as well as facilitated water dissociation and thus hydrogenation process. As a result, the Fe-HESA NCs exhibited a high selectivity toward NH3 from the electrocatalytic reduction of nitrate with a Faradaic efficiency of 93.4% while maintaining a high yield rate of 81.4 mg h−1 mg−1.

Suggested Citation

  • Sishuang Tang & Minghao Xie & Saerom Yu & Xun Zhan & Ruilin Wei & Maoyu Wang & Weixin Guan & Bowen Zhang & Yuyang Wang & Hua Zhou & Gengfeng Zheng & Yuanyue Liu & Jamie H. Warner & Guihua Yu, 2024. "General synthesis of high-entropy single-atom nanocages for electrosynthesis of ammonia from nitrate," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-51112-3
    DOI: 10.1038/s41467-024-51112-3
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    References listed on IDEAS

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    1. Nicolas Gruber & James N. Galloway, 2008. "An Earth-system perspective of the global nitrogen cycle," Nature, Nature, vol. 451(7176), pages 293-296, January.
    2. 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.
    3. 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.
    4. Xin Lei & Qingyun Tang & Yongping Zheng & Pinit Kidkhunthod & Xiaolong Zhou & Bifa Ji & Yongbing Tang, 2023. "High-entropy single-atom activated carbon catalysts for sustainable oxygen electrocatalysis," Nature Sustainability, Nature, vol. 6(7), pages 816-826, July.
    5. Bocheng Zhang & Zechuan Dai & Yanxu Chen & Mingyu Cheng & Huaikun Zhang & Pingyi Feng & Buqi Ke & Yangyang Zhang & Genqiang Zhang, 2024. "Defect-induced triple synergistic modulation in copper for superior electrochemical ammonia production across broad nitrate concentrations," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    6. Abhishek Sarkar & Leonardo Velasco & Di Wang & Qingsong Wang & Gopichand Talasila & Lea de Biasi & Christian Kübel & Torsten Brezesinski & Subramshu S. Bhattacharya & Horst Hahn & Ben Breitung, 2018. "High entropy oxides for reversible energy storage," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
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