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Ambient ammonia synthesis via palladium-catalyzed electrohydrogenation of dinitrogen at low overpotential

Author

Listed:
  • Jun Wang

    (University of Central Florida)

  • Liang Yu

    (Virginia Polytechnic Institute and State University)

  • Lin Hu

    (University of Central Florida)

  • Gang Chen

    (University of Central Florida)

  • Hongliang Xin

    (Virginia Polytechnic Institute and State University)

  • Xiaofeng Feng

    (University of Central Florida)

Abstract

Electrochemical reduction of N2 to NH3 provides an alternative to the Haber−Bosch process for sustainable, distributed production of NH3 when powered by renewable electricity. However, the development of such process has been impeded by the lack of efficient electrocatalysts for N2 reduction. Here we report efficient electroreduction of N2 to NH3 on palladium nanoparticles in phosphate buffer solution under ambient conditions, which exhibits high activity and selectivity with an NH3 yield rate of ~4.5 μg mg−1Pd h−1 and a Faradaic efficiency of 8.2% at 0.1 V vs. the reversible hydrogen electrode (corresponding to a low overpotential of 56 mV), outperforming other catalysts including gold and platinum. Density functional theory calculations suggest that the unique activity of palladium originates from its balanced hydrogen evolution activity and the Grotthuss-like hydride transfer mechanism on α-palladium hydride that lowers the free energy barrier of N2 hydrogenation to *N2H, the rate-limiting step for NH3 electrosynthesis.

Suggested Citation

  • Jun Wang & Liang Yu & Lin Hu & Gang Chen & Hongliang Xin & Xiaofeng Feng, 2018. "Ambient ammonia synthesis via palladium-catalyzed electrohydrogenation of dinitrogen at low overpotential," Nature Communications, Nature, vol. 9(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-04213-9
    DOI: 10.1038/s41467-018-04213-9
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    Cited by:

    1. Wenhui He & Jian Zhang & Stefan Dieckhöfer & Swapnil Varhade & Ann Cathrin Brix & Anna Lielpetere & Sabine Seisel & João R. C. Junqueira & Wolfgang Schuhmann, 2022. "Splicing the active phases of copper/cobalt-based catalysts achieves high-rate tandem electroreduction of nitrate to ammonia," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    2. Xinhong Chen & Yumeng Cheng & Bo Zhang & Jia Zhou & Sisi He, 2024. "Gradient-concentration RuCo electrocatalyst for efficient and stable electroreduction of nitrate into ammonia," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    3. Rao, Xufeng & Liu, Minmin & Chien, Meifang & Inoue, Chihiro & Zhang, Jiujun & Liu, Yuyu, 2022. "Recent progress in noble metal electrocatalysts for nitrogen-to-ammonia conversion," Renewable and Sustainable Energy Reviews, Elsevier, vol. 168(C).
    4. Santhosh, C.R. & Sankannavar, Ravi, 2023. "A comprehensive review on electrochemical green ammonia synthesis: From conventional to distinctive strategies for efficient nitrogen fixation," Applied Energy, Elsevier, vol. 352(C).
    5. Mushtaq, Muhammad Asim & Arif, Muhammad & Yasin, Ghulam & Tabish, Mohammad & Kumar, Anuj & Ibraheem, Shumaila & Ye, Wen & Ajmal, Saira & Zhao, Jie & Li, Pengyan & Liu, Jianfang & Saad, Ali & Fang, Xia, 2023. "Recent developments in heterogeneous electrocatalysts for ambient nitrogen reduction to ammonia: Activity, challenges, and future perspectives," Renewable and Sustainable Energy Reviews, Elsevier, vol. 176(C).
    6. Laihao Luo & Xinyan Liu & Xinyu Zhao & Xinyan Zhang & Hong-Jie Peng & Ke Ye & Kun Jiang & Qiu Jiang & Jie Zeng & Tingting Zheng & Chuan Xia, 2024. "Pressure-induced generation of heterogeneous electrocatalytic metal hydride surfaces for sustainable hydrogen transfer," Nature Communications, Nature, vol. 15(1), pages 1-15, December.

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