Yang Wenqiang, Liu Huan, Chang Xiaoxia, Zhang Yunlong, Cai Yafeng, Li Yifan, Cui Yi, Xu Bingjun, Yu Liang, Cui Xiaoju, Deng Dehui
State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China.
University of Chinese Academy of Sciences, Beijing, China.
Nat Commun. 2025 Feb 1;16(1):1257. doi: 10.1038/s41467-025-56548-9.
Electrocatalytic NO reduction reaction (NORR) offers a promising route for sustainable NH synthesis along with removal of NO pollutant. However, it remains a great challenge to accomplish both high NH production rate and long duration to satisfy industrial application demands. Here, we report an in situ-formed hierarchical porous Cu nanowire array monolithic electrode ensembled in a pressurized electrolyzer to regulate NORR reaction kinetics and thermodynamics, which delivers an industrial-level NH partial current density of 1007 mA cm with Faradaic efficiency of 96.1% and remains stable at 1000 mA cm for 100 hours. Integrating the Cu nanowire array monolithic electrode with pressurized electrolyzer boosts the NH production rate to 10.5 mmol h cm, which is over tenfold that using commercial Cu foam at 1 atm. The NORR performance can be attributed to the promoted NO mass transfer to the enriched Cu surface, which could increase the NO coverage on Cu and then destabilize adsorbed NO and weaken hydrogen adsorption, thereby facilitating NO hydrogenation to NH while suppressing the competing hydrogen evolution.
电催化NO还原反应（NORR）为可持续合成氨以及去除NO污染物提供了一条很有前景的途径。然而，要实现高氨产率和长反应持续时间以满足工业应用需求，仍然是一个巨大的挑战。在此，我们报道了一种原位形成的分级多孔铜纳米线阵列整体电极，其集成在一个加压电解槽中以调节NORR反应动力学和热力学，该电极实现了1007 mA cm的工业级氨分电流密度，法拉第效率为96.1%，并在1000 mA cm下保持稳定100小时。将铜纳米线阵列整体电极与加压电解槽相结合，将氨产率提高到10.5 mmol h cm，这是在1个大气压下使用商业泡沫铜时产率的十倍以上。NORR性能可归因于促进了NO向富集铜表面的传质，这可以增加NO在铜上的覆盖度，进而使吸附的NO不稳定并减弱氢吸附，从而促进NO加氢生成氨，同时抑制竞争性析氢反应。
