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Identifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst

Author

Listed:
  • Xiaoran Zhang

    (Hunan University
    Curtin University)

  • Xiaorong Zhu

    (Nanjing Normal University)

  • Shuowen Bo

    (University of Science and Technology of China)

  • Chen Chen

    (Hunan University)

  • Mengyi Qiu

    (Hunan University)

  • Xiaoxiao Wei

    (Hunan University)

  • Nihan He

    (Hunan University)

  • Chao Xie

    (Hunan University)

  • Wei Chen

    (Hunan University)

  • Jianyun Zheng

    (Hunan University)

  • Pinsong Chen

    (Curtin University)

  • San Ping Jiang

    (Curtin University
    Foshan Xianhu Laboratory of the Advanced Energy Science and Technology Guangdong Laboratory)

  • Yafei Li

    (Nanjing Normal University)

  • Qinghua Liu

    (University of Science and Technology of China)

  • Shuangyin Wang

    (Hunan University)

Abstract

Electrocatalytic urea synthesis emerged as the promising alternative of Haber–Bosch process and industrial urea synthetic protocol. Here, we report that a diatomic catalyst with bonded Fe–Ni pairs can significantly improve the efficiency of electrochemical urea synthesis. Compared with isolated diatomic and single-atom catalysts, the bonded Fe–Ni pairs act as the efficient sites for coordinated adsorption and activation of multiple reactants, enhancing the crucial C–N coupling thermodynamically and kinetically. The performance for urea synthesis up to an order of magnitude higher than those of single-atom and isolated diatomic electrocatalysts, a high urea yield rate of 20.2 mmol h−1 g−1 with corresponding Faradaic efficiency of 17.8% has been successfully achieved. A total Faradaic efficiency of about 100% for the formation of value-added urea, CO, and NH3 was realized. This work presents an insight into synergistic catalysis towards sustainable urea synthesis via identifying and tailoring the atomic site configurations.

Suggested Citation

  • Xiaoran Zhang & Xiaorong Zhu & Shuowen Bo & Chen Chen & Mengyi Qiu & Xiaoxiao Wei & Nihan He & Chao Xie & Wei Chen & Jianyun Zheng & Pinsong Chen & San Ping Jiang & Yafei Li & Qinghua Liu & Shuangyin , 2022. "Identifying and tailoring C–N coupling site for efficient urea synthesis over diatomic Fe–Ni catalyst," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
  • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33066-6
    DOI: 10.1038/s41467-022-33066-6
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    1. Mengqiu Xu & Fangfang Wu & Ye Zhang & Yuanhui Yao & Genping Zhu & Xiaoyu Li & Liang Chen & Gan Jia & Xiaohong Wu & Youju Huang & Peng Gao & Wei Ye, 2023. "Kinetically matched C–N coupling toward efficient urea electrosynthesis enabled on copper single-atom alloy," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Qian Wu & Chencheng Dai & Fanxu Meng & Yan Jiao & Zhichuan J. Xu, 2024. "Potential and electric double-layer effect in electrocatalytic urea synthesis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    3. Yilong Zhao & Yunxuan Ding & Wenlong Li & Chang Liu & Yingzheng Li & Ziqi Zhao & Yu Shan & Fei Li & Licheng Sun & Fusheng Li, 2023. "Efficient urea electrosynthesis from carbon dioxide and nitrate via alternating Cu–W bimetallic C–N coupling sites," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Han Li & Leitao Xu & Shuowen Bo & Yujie Wang & Han Xu & Chen Chen & Ruping Miao & Dawei Chen & Kefan Zhang & Qinghua Liu & Jingjun Shen & Huaiyu Shao & Jianfeng Jia & Shuangyin Wang, 2024. "Ligand engineering towards electrocatalytic urea synthesis on a molecular catalyst," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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