Research Article

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2022, 15(2): 1039–1046

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https://doi.org/10.1007/s12274-021-3592-8

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

Tong Xu1,2,§, Jie Liang1,§, Yuanyuan Wang3, Shaoxiong Li1, Zhaobai Du1, Tingshuai Li1, Qian Liu4, Yonglan Luo4, Fang Zhang5, Xifeng Shi6, Bo Tang6, Qingquan Kong4, Abdullah M. Asiri7, Chun Yang2 (✉), Dongwei Ma3 (✉), and Xuping Sun1 (✉)

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1 Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, China
2 College of Chemistry and Materials Science, Sichuan Normal University, Chengdu 610068, China
3 Key Laboratory for Special Functional Materials of Ministry of Education, and School of Materials Science and Engineering, Henan University, Kaifeng 475004, China
4 Institute for Advanced Study, Chengdu University, Chengdu 610106, China
5 National Engineering Research Center for Nanotechnology, No. 28 East Jiang Chuan Road, Shanghai 200241, China
6 College of Chemistry, Chemical Engineering and Materials Science, Shandong Normal University, Jinan 250014, China
7 Chemistry Department, Faculty of Science & Center of Excellence for Advanced Materials Research, King Abdulaziz University, P.O. Box 80203, Jeddah 21589, Saudi Arabia
§ Tong Xu and Jie Liang contributed equally to this work.

Keywords: Fe3P nanoarrays, octadecanethiol, surface modification, ambient N2 reduction, first-principles calculation
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  • Abstract
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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 octadecanethiolmodified 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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Enhancing electrocatalytic N2-to-NH3 fixation by suppressing hydrogen evolution with alkylthiols modified Fe3P nanoarrays. Nano Res. 2022, 15(2): 1039–1046 https://doi.org/10.1007/s12274-021-3592-8

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