Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, Guangdong 518055, People's Republic of China.
Department of Chemical and Biological Engineering, The Hong Kong University of Science and Technology, Clear Water Bay, Kowloon, Hong Kong 999077, People's Republic of China.
Nano Lett. 2023 Mar 8;23(5):1897-1903. doi: 10.1021/acs.nanolett.2c04949. Epub 2023 Feb 22.
The electrochemical nitrate reduction reaction (NORR) is a promising alternative synthetic route for sustainable ammonia (NH) production, because it not only eliminates nitrate (NO) from water but also produces NH under mild operating conditions. However, owing to the complicated eight-electron reaction and the competition from the hydrogen evolution reaction, developing catalysts with high activities and Faradaic efficiencies (FEs) is highly imperative to improve the reaction performance. In this study, Cu-doped FeO flakes are fabricated and demonstrated to be excellent catalysts for electrochemical conversion of NO to NH, with a maximum FE of ∼100% and an NH yield of 179.55 ± 16.37 mg h mg at -0.6 V vs RHE. Theoretical calculations reveal that doping the catalyst surface with Cu results in a more thermodynamically facile reaction. These results highlight the feasibility of promoting the NORR activity using heteroatom doping strategies.
电化学硝酸盐还原反应(NORR)是一种很有前途的可持续氨(NH)生产的替代合成途径,因为它不仅可以从水中消除硝酸盐(NO),而且可以在温和的操作条件下产生 NH。然而,由于复杂的八电子反应和析氢反应的竞争,开发具有高活性和法拉第效率(FE)的催化剂对于提高反应性能至关重要。在这项研究中,制备了掺铜的 FeO 薄片,并证明其是电化学将 NO 转化为 NH 的优异催化剂,在 -0.6 V 相对于 RHE 的电位下,最大 FE 约为 100%,NH 产率为 179.55 ± 16.37 mg h mg。理论计算表明,在催化剂表面掺杂 Cu 会导致更热力学上容易的反应。这些结果突出了使用杂原子掺杂策略来促进 NORR 活性的可行性。