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Selective electrocatalytic synthesis of urea with nitrate and carbon dioxide

Author

Listed:
  • Chade Lv

    (Nanyang Technological University)

  • Lixiang Zhong

    (Nanyang Technological University)

  • Hengjie Liu

    (University of Science and Technology of China)

  • Zhiwei Fang

    (The University of Texas at Austin)

  • Chunshuang Yan

    (Nanyang Technological University
    School of Chemistry and Chemical Engineering, Harbin Institute of Technology)

  • Mengxin Chen

    (Nanyang Technological University)

  • Yi Kong

    (School of Chemistry and Chemical Engineering, Harbin Institute of Technology)

  • Carmen Lee

    (Nanyang Technological University)

  • Daobin Liu

    (Nanyang Technological University)

  • Shuzhou Li

    (Nanyang Technological University)

  • Jiawei Liu

    (Nanyang Technological University)

  • Li Song

    (University of Science and Technology of China)

  • Gang Chen

    (School of Chemistry and Chemical Engineering, Harbin Institute of Technology)

  • Qingyu Yan

    (Nanyang Technological University)

  • Guihua Yu

    (The University of Texas at Austin)

Abstract

Synthetic nitrogen fertilizer such as urea has been key to increasing crop productivity and feeding a growing population. However, the conventional urea production relies on energy-intensive processes, consuming approximately 2% of annual global energy. Here, we report on a more-sustainable electrocatalytic approach that allows for direct and selective synthesis of urea from nitrate and carbon dioxide with an indium hydroxide catalyst at ambient conditions. Remarkably, Faradaic efficiency, nitrogen selectivity and carbon selectivity reach 53.4%, 82.9% and ~100%, respectively. The engineered surface semiconducting behaviour of the catalyst is found to suppress hydrogen evolution reaction. The key step of C–N coupling initiates through the reaction between *NO2 and *CO2 intermediates owing to the low energy barrier on {100} facets. This work suggests an appealing route of urea production and provides deep insight into the underlying chemistry of C–N coupling reaction that could guide sustainable synthesis of other indispensable chemicals.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natsus:v:4:y:2021:i:10:d:10.1038_s41893-021-00741-3
    DOI: 10.1038/s41893-021-00741-3
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    Citations

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    Cited by:

    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. Bharath, G. & Karthikeyan, G. & Kumar, Anuj & Prakash, J. & Venkatasubbu, Devanand & Kumar Nadda, Ashok & Kumar Gupta, Vijai & Abu Haija, Mohammad & Banat, Fawzi, 2022. "Surface engineering of Au nanostructures for plasmon-enhanced electrochemical reduction of N2 and CO2 into urea in the visible-NIR region," Applied Energy, Elsevier, vol. 318(C).
    3. 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.
    4. Kui Fan & Wenfu Xie & Jinze Li & Yining Sun & Pengcheng Xu & Yang Tang & Zhenhua Li & Mingfei Shao, 2022. "Active hydrogen boosts electrochemical nitrate reduction to ammonia," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    5. 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.
    6. Yurou Celine Xiao & Siyu Sonia Sun & Yong Zhao & Rui Kai Miao & Mengyang Fan & Geonhui Lee & Yuanjun Chen & Christine M. Gabardo & Yan Yu & Chenyue Qiu & Zunmin Guo & Xinyue Wang & Panagiotis Papangel, 2024. "Reactive capture of CO2 via amino acid," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    7. Yang Li & Shisheng Zheng & Hao Liu & Qi Xiong & Haocong Yi & Haibin Yang & Zongwei Mei & Qinghe Zhao & Zu-Wei Yin & Ming Huang & Yuan Lin & Weihong Lai & Shi-Xue Dou & Feng Pan & Shunning Li, 2024. "Sequential co-reduction of nitrate and carbon dioxide enables selective urea electrosynthesis," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    8. 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.
    9. 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.
    10. 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.

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