Capturing Copper Single Atom in Proton Donor Stimulated O‐End Nitrate Reduction
Yunpeng Zuo, Mingzi Sun, Tingting Li, Libo Sun, Shuhe Han, Yang Chai, Bolong Huang, Xin Wang
Abstract
Abstract Ammonia (NH 3 ) is vital in global production and energy cycles. Electrocatalytic nitrate reduction (e‐NO 3 RR) offers a promising route for nitrogen (N) conversion and NH 3 synthesis, yet it faces challenges like competing reactions and low catalyst activity. This study proposes a synergistic mechanism incorporating a proton donor to mediate O‐end e‐NO 3 RR, addressing these limitations. A novel method combining ultraviolet radiation reduction, confined synthesis, and microwave treatment was developed to create a model catalyst embedding Cu single atoms on La‐based nanoparticles ( p ‐CNCu s La n ‐m). DFT analysis emphasizes the critical role of La‐based clusters as proton donors in e‐NO 3 RR, while in situ characterization reveals an O‐end adsorption reduction mechanism. The catalyst achieves a remarkable Faraday efficiency (FE NH3 ) of 97.7%, producing 10.6 mol g metal −1 h −1 of NH 3 , surpassing most prior studies. In a flow cell, it demonstrated exceptional stability, with only a 9% decrease in current density after 111 hours and a NH 3 production rate of 1.57 mg NH3 /h/cm −2 . The proton donor mechanism's effectiveness highlights its potential for advancing electrocatalyst design. Beyond NH 3 production, the O‐end mechanism opens avenues for exploring molecular‐oriented coupling reactions in e‐NO 3 RR, paving the way for innovative electrochemical synthesis applications.