Boosting Electrocatalytic Ammonia Synthesis via Synergistic Effect of Iron-Based Single Atoms and Clusters.
Boosting Electrocatalytic Ammonia Synthesis via Synergistic Effect of Iron-Based Single Atoms and Clusters.
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DOI：
10.1021/acs.nanolett.3c04049
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发表时间：
2024-01
期刊：
影响因子：
10.8
通讯作者：
Li Xu;Tong Liu;Dong Liu;Airong Xu;Sicong Wang;Hui Huang;Xiaokang Liu;Mei Sun;Q. Luo;Xusheng Zheng;Tao Ding;Tao Yao
中科院分区：
文献类型：
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作者：
Li Xu;Tong Liu;Dong Liu;Airong Xu;Sicong Wang;Hui Huang;Xiaokang Liu;Mei Sun;Q. Luo;Xusheng Zheng;Tao Ding;Tao Yao
电催化还原硝态氮制氨（NO3RR）是一种低碳、环保的工艺。然而，氨收率低和选择性差仍然是该多质子偶联工艺的主要挑战。在此，我们报告了一种由Fe单原子和Fe3C原子团簇组成的新型Fe基杂化结构的简单策略，该结构在协同电催化NO3RR方面表现出出色的性能。通过operando同步傅里叶变换红外光谱和理论计算，我们明确了Fe单原子是NO3RR的活性位点，而Fe3C簇促进H2O解离，为持续的氢化反应提供质子（*H）。结果表明，铁基电催化剂的氨法拉第效率接近100%，在-0.4 V vs RHE下，相应的产率为24768 μg h-1 cm-2，超过了大多数金属基催化剂。本研究为多步反应提供了有价值的指导。
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.