Fe3C纳米晶体电催化一氧化氮还原合成氨

doi:10.61558/2993-074X.3525

电化学（中英文） ›› 2025, Vol. 31 ›› Issue (4): 2412171. doi: 10.61558/2993-074X.3525

Fe₃C纳米晶体电催化一氧化氮还原合成氨

林森^a, 张浪^a, 侯童^a^,^*(), 丁俊阳^a, 彭紫默^a^,^*(), 刘亦帆^b, 刘熙俊^a^,^*()

^a广西大学资源环境与材料学院，广西有色金属及特色材料加工重点实验室，省部共建特色金属材料与组合结构全寿命安全国家重点实验室，广西南宁 530004
^b苏州实验室，江苏苏州 21510

收稿日期:2024-12-17 接受日期:2025-02-08 发布日期:2025-02-15 出版日期:2025-04-28
通讯作者: 侯童,彭紫默,刘熙俊 E-mail:houtong3393@163.com;18944614368@163.com;xjliu@gxu.edu.cn

Electrocatalytic Nitric Oxide Reduction to Yield Ammonia over Fe₃C Nanocrystals

Lin Sen^a, Zhang Lang^a, Hou Tong^a^,^*(), Ding Jun-Yang^a, Peng Zi-Mo^a^,^*(), Liu Yi-Fan^b, Liu Xi-Jun^a^,^*()

^aState Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures, Guangxi Key Laboratory of Processing for Non-ferrous Metals and Featured Materials, School of Resources, Environment and Materials, Guangxi University, Nanning 530004, Guangxi, China
^bSuzhou Laboratory, Suzhou 215100, Jiangsu, China

Received:2024-12-17 Accepted:2025-02-08 Online:2025-02-15 Published:2025-04-28
Contact: Hou Tong, Peng Zi-Mo, Liu Xi-Jun E-mail:houtong3393@163.com;18944614368@163.com;xjliu@gxu.edu.cn
About author:First author contact:^#These authors contributed equally to this work.

1. 2412171-Electrocatalytic Nitric Oxide Reduction to Yield Ammonia over Fe3C Nanocrystals-Supporting information.pdf(2536KB)

摘要/Abstract

摘要：

一氧化氮（NO）通常来自汽车尾气和工业烟气，是最严重的空气污染物之一。为解决这一问题，电催化一氧化氮还原反应（NORR）被提出，其不仅能去除NO大气污染物，还能产生有价值的氨（NH₃）。因此，通过对Fe₃C纳米晶体进行改性，制备的Fe₃C/C-900样品在常温常压条件下可作为高效NORR催化剂。电化学测试结果表明，Fe₃C/C-900催化剂在-0.8 V（vs. RHE）时的合成NH₃法拉第效率为76.5%，在-1.2 V（vs. RHE）时的NH₃产率为177.5 μmol·h^-1·cm^-2。同时，其在长时间电解过程中，也能保持稳定的NORR活性。此外，我们将Fe₃C/C-900的高NORR特性归因于两个方面：一方面，Fe₃C纳米晶体的内在活性，包括降低决速步骤（*NOH→*N）能垒和抑制氢析出副反应；另一方面，多孔碳基底有利于活性成分的分散、气态NO反应物的有效吸附和液态NH₃产物的释放。

关键词: 一氧化氮还原, 合成氨, Fe₃C纳米晶体, 电催化, 理论计算

Abstract:

Nitric oxide (NO), which generally originates from vehicle exhaust and industrial flue gases, is one of the most serious air pollutants. In this case, the electrochemical NO reduction reaction (NORR) not only removes the atmospheric pollutant NO but also produces valuable ammonia (NH₃). Hence, through the synthesis and modification of Fe₃C nanocrystal catalysts, the as-obtained optimal sample of Fe₃C/C-900 was adopted as the NORR catalyst at ambient conditions. As a result, the Fe₃C/C-900 catalyst showed an NH₃ Faraday efficiency of 76.5% and an NH₃ yield rate of 177.5 μmol·h^-1·cm^-2 at the working potentials of -0.8 and -1.2 V versus reversible hydrogen electrode (vs. RHE), respectively. And it delivered a stable NORR activity during the electrolysis. Moreover, we attribute the high NORR properties of Fe₃C/C-900 to two aspects: one is the enhanced intrinsic activity of Fe₃C nanocrystals, including the lowering of the energy barrier of rate-limiting step (*NOH→*N) and the inhibition of hydrogen evolution; on the other hand, the favorable dispersion of active components, the effective adsorption of gaseous NO, and the release of liquid NH₃ products facilitated by the porous carbon substrate.

Key words: Nitric oxide reduction, NH₃ synthesis, Fe₃C nanocrystal, Electrolysis, Theoretical calculation

林森, 张浪, 侯童, 丁俊阳, 彭紫默, 刘亦帆, 刘熙俊. Fe₃C纳米晶体电催化一氧化氮还原合成氨[J]. 电化学（中英文）, 2025, 31(4): 2412171.

Lin Sen, Zhang Lang, Hou Tong, Ding Jun-Yang, Peng Zi-Mo, Liu Yi-Fan, Liu Xi-Jun. Electrocatalytic Nitric Oxide Reduction to Yield Ammonia over Fe₃C Nanocrystals[J]. Journal of Electrochemistry, 2025, 31(4): 2412171.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.61558/2993-074X.3525

https://electrochem.xmu.edu.cn/CN/Y2025/V31/I4/2412171

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参考文献 32

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Fe₃C纳米晶体电催化一氧化氮还原合成氨

Electrocatalytic Nitric Oxide Reduction to Yield Ammonia over Fe₃C Nanocrystals

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