A Reaction-Diffusion-Coupled Strategy for Ampere-Level Electrocatalytic Nitrate Reduction to Ammonia

作者：Shurong Li, Yiwen Su, Hao Wan, Zheng Jiang, Tianhao Niu, Yong Zhang, Wei Huang, Libin Zeng, Haiqing Zhou, Guangping Zheng, Zhong‐Zhen Yu, Jingyu Sun, Jing Yang, Shi Xue Dou · 发表于：Nano Letters · 年份：2025 · DOI：10.1021/acs.nanolett.5c03905 · 被引用次数：8 · 研究领域：Ammonia Synthesis and Nitrogen Reduction、Hydrogen Storage and Materials、Muon and positron interactions and applications

Ampere-level electrocatalytic nitrate reduction to ammonia (eNRA) offers a carbon-neutral alternative to the Haber–Bosch process. However, its energy efficiency is critically hampered by the inherent conflict between the reaction and diffusion. Herein, we propose a reaction-diffusion-coupled strategy implemented on a well-tailored CuCoNiRuPt high-entropy alloy aerogel (HEAA) to simultaneously realize energy barrier homogenization and accelerate mass transport, endowing ampere-level eNRA with a high energy efficiency. The resultant HEAA delivers an ammonia yield rate of 3.4 ± 0.3 mmol·h –1 ·cm –2 and a Faradaic efficiency of 98 ± 2% at a record-low overpotential of −0.05 V versus a reversible hydrogen electrode, enabling an energy efficiency of 41.5 ± 0.8% and a durable operation at industrial current density. Pragmatic deployment is further envisaged in a membrane electrode assembly electrolyzer to achieve practical-scale ammonia production with a yield rate of 4.3 ± 0.1 mmol·h –1 ·cm –2 at 1 A·cm –2 . This work pioneers new pathways for developing efficient catalysts toward the industrial application of eNRA.