电催化剂
氨生产
法拉第效率
催化作用
离解(化学)
氨
化学
同步加速器
电化学
无机化学
材料科学
电极
物理化学
生物化学
物理
有机化学
核物理学
作者
Li Xu,Tong Liu,Dong Liu,Airong Xu,Sicong Wang,Hui Hu,Xiaokang Liu,Min Sun,Qiquan Luo,Xusheng Zheng,Tao Ding,Takeshi Yao
出处
期刊:Nano Letters
[American Chemical Society]
日期:2024-01-16
卷期号:24 (4): 1197-1204
标识
DOI:10.1021/acs.nanolett.3c04049
摘要
Electrocatalytic reduction of nitrate to ammonia (NO3RR) is gaining attention for low carbon emissions and environmental protection. However, low ammonia production rate and poor selectivity have remained major challenges in this multi-proton coupling process. Herein, we report a facile strategy toward a novel Fe-based hybrid structure composed of Fe single atoms and Fe3C atomic clusters that demonstrates outstanding performance for synergistic electrocatalytic NO3RR. By operando synchrotron Fourier transform infrared spectroscopy and theoretical computation, we clarify that Fe single atoms serve as the active site for NO3RR, while Fe3C clusters facilitate H2O dissociation to provide protons (*H) for continued hydrogenation reactions. As a result, the Fe-based electrocatalyst exhibits ammonia Faradaic efficiency of nearly 100%, with a corresponding production rate of 24768 μg h–1 cm–2 at −0.4 V vs RHE, exceeding most reported metal-based catalysts. This research provides valuable guidance toward multi-step reactions.
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