Li Tingsong, Tang Chun, Guo Heng, Wu Haoran, Duan Chao, Wang Hao, Zhang Fengying, Cao Yuehan, Yang Guidong, Zhou Ying
State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu610500, China.
School of New Energy and Materials, Southwest Petroleum University, Chengdu610500, China.
ACS Appl Mater Interfaces. 2022 Oct 25. doi: 10.1021/acsami.2c14215.
Electrochemical reduction of nitrate to ammonia (NH), a green NH production route upon combining with renewable energy sources, is an appealing and alternative method to the Haber-Bosch process. However, this process not only involves the complicated eight-electron reduction to transform nitrate into various nitrogen products but simultaneously suffers from the competitive hydrogen evolution reaction, challenged by a lack of efficient catalysts. Herein, the growth of FeO nanorod arrays on carbon cloth (FeO NRs/CC) is reported to exhibit a high NH yield rate of 328.17 μmol h cm at -0.9 V versus RHE, outperforming most of the reported Fe catalysts. An growth strategy provides massive exposed active sites and a fast electron-transport channel between the carbon cloth and FeO, which accelerates the charge-transport rate and facilitates the conversion of nitrate to NH. Raman spectroscopy in conjunction with attenuated total reflection Fourier transform infrared spectroscopy reveals the catalytic mechanism of nitrate to NH. Our study provides not only an efficient catalyst for NH production but also useful guidelines for the pathways and mechanism of nitrate electroreduction to NH.
将硝酸盐电化学还原为氨（NH₃），这一与可再生能源相结合的绿色氨生产途径，是哈伯-博施法颇具吸引力的替代方法。然而，该过程不仅涉及将硝酸盐转化为各种氮产物的复杂八电子还原反应，同时还受到竞争性析氢反应的影响，且缺乏高效催化剂也构成挑战。在此，据报道在碳布上生长的FeO纳米棒阵列（FeO NRs/CC）在相对于可逆氢电极（RHE）为-0.9 V时表现出328.17 μmol h⁻¹ cm⁻²的高氨产率，优于大多数已报道的铁催化剂。一种生长策略提供了大量暴露的活性位点以及碳布与FeO之间快速的电子传输通道，这加速了电荷传输速率并促进了硝酸盐向氨的转化。拉曼光谱结合衰减全反射傅里叶变换红外光谱揭示了硝酸盐转化为氨的催化机理。我们的研究不仅为氨生产提供了一种高效催化剂，还为硝酸盐电还原为氨的途径和机理提供了有用的指导。
