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Enhancing electrocatalytic N2-to-NH3 fixation by suppressing hydrogen evolution with alkylthiols modified Fe3P nanoarrays

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Abstract

Electrocatalytic N2 reduction provides an attractive alternative to Haber-Bosch process for artificial NH3 synthesis. The difficulty of suppressing competing proton reduction, however, largely impedes its practical use. Herein, we design a hydrophobic octadecanethiol-modified Fe3P nanoarrays supported on carbon paper (C18@Fe3P/CP) to effectively repel water, concentrate N2, and enhance N2-to-NH3 conversion. Such catalyst achieves an NH3 yield of 1.80 × 10−10 mol·s−1·cm−2 and a high Faradaic efficiency of 11.22% in 0.1 M Na2SO4, outperforming the non-modified Fe3P/CP (2.16 × 10−11 mol·s−1·cm−2, 0.9%) counterpart. Significantly, C18@Fe3P/CP renders steady N2-fixing activity/selectivity in cycling test and exhibits durability for at least 25 h. First-principles calculations suggest that the surface electronic structure and chemical activity of Fe3P can be well tuned by the thiol modification, which facilitates N2 electroreduction activity and catalytic formation of NH3.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (No. 22072015), Shanghai Scientific and Technological Innovation Project (No. 18JC 1410604), and Program for Science & Technology Innovation Talents in Universities of Henan Province (No. 20HASTIT028).

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  1. Tong Xu and Jie Liang contributed equally to this work.

Authors and Affiliations

  1. Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu, 610054, China

    Tong Xu, Jie Liang, Shaoxiong Li, Zhaobai Du, Tingshuai Li & Xuping Sun

  2. College of Chemistry and Materials Science, Sichuan Normal University, Chengdu, 610068, China

    Tong Xu & Chun Yang

  3. Key Laboratory for Special Functional Materials of Ministry of Education, and School of Materials Science and Engineering, Henan University, Kaifeng, 475004, China

    Yuanyuan Wang & Dongwei Ma

  4. Institute for Advanced Study, Chengdu University, Chengdu, 610106, China

    Qian Liu, Yonglan Luo & Qingquan Kong

  5. National Engineering Research Center for Nanotechnology, No. 28 East Jiang Chuan Road, Shanghai, 200241, China

    Fang Zhang

  6. College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan, 250014, China

    Xifeng Shi & Bo Tang

  7. Chemistry Department, Faculty of Science & Center of Excellence for Advanced Materials Research, King Abdulaziz University, P.O. Box 80203, Jeddah, 21589, Saudi Arabia

    Abdullah M. Asiri

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  1. Tong Xu
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Correspondence to Chun Yang, Dongwei Ma or Xuping Sun.

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Enhancing electrocatalytic N2-to-NH3 fixation by suppressing hydrogen evolution with alkylthiols modified Fe3P nanoarrays

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Xu, T., Liang, J., Wang, Y. et al. Enhancing electrocatalytic N2-to-NH3 fixation by suppressing hydrogen evolution with alkylthiols modified Fe3P nanoarrays. Nano Res. 15, 1039–1046 (2022). https://doi.org/10.1007/s12274-021-3592-8

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