Authors: Yunpeng Zuo, Mingzi Sun, Tingting Li, Libo Sun, Shuhe Han, Yang Chai, Bolong Huang, Xin Wang
Published: 2025-02-19
Source: Full article
AbstractAmmonia (NH3) is vital in global production and energy cycles. Electrocatalytic nitrate reduction (e‐NO3RR) offers a promising route for nitrogen (N) conversion and NH3 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‐NO3RR, 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‐CNCusLan‐m). DFT analysis emphasizes the critical role of La‐based clusters as proton donors in e‐NO3RR, while in situ characterization reveals an O‐end adsorption reduction mechanism. The catalyst achieves a remarkable Faraday efficiency (FENH3) of 97.7%, producing 10.6 mol gmetal−1 h−1 of NH3, 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 NH3 production rate of 1.57 mgNH3/h/cm−2. The proton donor mechanism's effectiveness highlights its potential for advancing electrocatalyst design. Beyond NH3 production, the O‐end mechanism opens avenues for exploring molecular‐oriented coupling reactions in e‐NO3RR, paving the way for innovative electrochemical synthesis applications.