Electrochemical NO₂⁻-to-NH₃ conversion (NO₂RR) offers a green route to NH₃ electrosynthesis, while developing efficient NO₂RR catalysis systems at high current densities remains a grand challenge. Herein, we report an efficient Zr-NiO catalyst with atomically dispersed Zr-dopants incorporated in NiO lattice, delivering the exceptional NO₂RR performance with industrial-level current density (>0.2 A cm⁻²). In situ spectroscopic measurements and theoretical simulations reveal the construction of Zr-Ni frustrated Lewis acid-base pairs (FLPs) on Zr-NiO, which can substantially increase the number of absorbed nitrite (NO₂⁻), promote the activation and protonation of NO₂⁻ and concurrently hamper the H coverage, boosting the activity and selectivity of Zr-NiO towards the NO₂RR. Remarkably, Zr-NiO exhibits the exceptional performance in a flow cell with high Faradaic efficiency for NH₃ of 94.0% and NH₃ yield rate of 1,394.1 µmol h⁻¹ cm⁻² at an industrial-level current density of 228.2 mA cm⁻², placing it among the best NO₂RR electrocatalysts for NH₃ production.

电化学NO ₂ ^-至NH ₃转化（NO _{2 RR）为NH 3}电合成提供了一条绿色途径，而在高电流密度下开发高效的NO ₂ RR催化系统仍然是一个巨大的挑战。在此，我们报道了一种高效的Zr-NiO催化剂，其在NiO晶格中加入了原子分散的Zr掺杂剂，可提供卓越的NO ₂ RR性能和工业级电流密度（>0.2 A cm ^-2）。原位光谱测量和理论模拟揭示了Zr-NiO上Zr-Ni受挫路易斯酸碱对（FLP）的构建，可以大幅增加吸收的亚硝酸盐（NO ₂ ^-）的数量，促进NO的活化和质子化₂ ^{−同时阻碍 H 覆盖，提高 Zr-NiO 对 NO} ₂ RR的活性和选择性。值得注意的是，Zr-NiO在流通池中表现出优异的性能，在228.2 mA cm ^-2的工业级电流密度下， NH _{3 的}法拉第效率高达94.0%，NH ₃产率为1,394.1 µmol h ^-1 cm ^{-2 。 ，使其成为用于 NH} ₃生产的最佳 NO ₂ RR 电催化剂之一。