Zhang Kouer, Xu Yifan, Liu Fatang, Wang Qing, Zou Xiaohong, Tang Mingcong, Leung Michael K H, Ao Zhimin, Zhao Xunhua, Zhang Xiao, An Liang
Department of Mechanical Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong Kong SAR, 999077, China.
Ability R&D Energy Research Centre, School of Energy and Environment, City University of Hong Kong, Kowloon, Hong Kong SAR, 999077, China.
Adv Sci (Weinh). 2025 Jan;12(4):e2410763. doi: 10.1002/advs.202410763. Epub 2024 Dec 2.
The efficiency of nitrate reduction reaction (NORR) at low nitrate concentration is predominantly hindered by the poor affinity of nitrate ions and competitive hydrogen evolution reaction (HER), particularly in neutral and acidic media. Here, an innovative strategy to leverage the interfacial electric field (IEF) is introduced to boost the NORR performance. By in situ constructing tannic acid-metal ion (TA-M) crosslinked structure on the electrode surface, the TA-M-CuO NW/Cu foam sample exhibits an exceptional Faraday efficiency of 99.4% at -0.2 V versus reversible hydrogen electrode (RHE) and 83.9% at 0.0 V versus RHE under neutral and acidic conditions, respectively. The computational studies unveil that the TA-Cu complex on the CuO (111) plane induces the increasing concentration of nitrate at the interface, accelerating NORR kinetics over HER via the IEF effect. This interfacial modulation strategy also contributes the enhanced ammonia production performance when it is employed on commercial electrode materials and flow reactors, exhibiting great potential in practical application. Overall, combined results illustrated multiple merits of the IEF effect, paving the way for future commercialization of NORR in the ammonia production industry.
在低硝酸盐浓度下,硝酸盐还原反应(NORR)的效率主要受到硝酸根离子亲和力差和竞争性析氢反应(HER)的阻碍,尤其是在中性和酸性介质中。在此,引入了一种利用界面电场(IEF)的创新策略来提高NORR性能。通过在电极表面原位构建单宁酸-金属离子(TA-M)交联结构,TA-M-CuO NW/Cu泡沫样品在相对于可逆氢电极(RHE)为-0.2 V时表现出99.4%的优异法拉第效率,在中性和酸性条件下,相对于RHE为0.0 V时分别为83.9%。计算研究表明,CuO(111)平面上的TA-Cu络合物会导致界面处硝酸盐浓度增加,通过IEF效应加速NORR动力学而非HER。当这种界面调制策略应用于商业电极材料和流动反应器时,也有助于提高氨生产性能,在实际应用中显示出巨大潜力。总体而言,综合结果说明了IEF效应的多个优点,为NORR在氨生产行业的未来商业化铺平了道路。