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Surface-Enhanced Raman Spectroscopic Study of Key Intermediates in Electrochemical Ammonia Decomposition
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-12-26 , DOI: 10.1021/jacs.4c15489
Xiaomeng Du, Aoxuan Du, Dan Wang, Yue Mao, Zhao Zhang, Wei Xie

Ammonia is an alternative hydrogen storage material and a promising source of sustainable clean energy. The lack of a mechanistic understanding of ammonia electrooxidation hinders the efforts to overcome the slow kinetics of the anode reaction in direct ammonia fuel cells. Herein, we use surface-enhanced Raman spectroscopy to study the electro-decomposition of ammonia on the Au surface. We observe three key reaction intermediate species of *NH2, *NH and *NNH and thereby disclose a multistage interfacial decomposition mechanism. Among the three, detection of the N-coupled species fills the blank in the mechanistic study of ammonia oxidation. Additionally, we investigated the influence of the reactant concentrations on the different oxidation stages. This spectroscopic evidence opens up promising avenues to overcome the limitations associated with ammonia fuel cells.

中文翻译:


电化学氨分解中关键中间体的表面增强拉曼光谱研究



氨是一种替代储氢材料,也是可持续清洁能源的有前途的来源。缺乏对氨电氧化机理的理解阻碍了克服直接氨燃料电池中阳极反应缓慢动力学的努力。在此,我们使用表面增强拉曼光谱来研究氨在 Au 表面的电分解。我们观察到 *NH2、*NH 和 *NNH 的三种关键反应中间体,从而揭示了多级界面分解机制。在这三者中,N 偶联物质的检测填补了氨氧化机理研究的空白。此外,我们还研究了反应物浓度对不同氧化阶段的影响。这些光谱证据为克服与氨燃料电池相关的限制开辟了有希望的途径。
更新日期:2024-12-27
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