文献类型：期刊文献

英文题名：Tandem electrocatalytic nitrate reduction to ammonia on a Cu/Fe(OH)3 heterostructure via dual-active sites synergy

作者：Xu, Wenxuan[1,2,4];Meng, Guangyuan[2,4];Zhang, Xinwan[2,4];Yin, Di[3];Qiu, Yannan[2,4];Zhang, Lehua[1,2,4];Liao, Benren[5];Jia, Daqing[2,4]

机构：[1]Shihezi Univ, Sch Chem & Chem Engn, Shihezi 832003, Xinjiang, Peoples R China;[2]East China Univ Sci & Technol, Natl Engn Res Ctr Ind Wastewater Detoxicat & Resou, Shanghai 200237, Peoples R China;[3]City Univ Hong Kong, Dept Mat Sci & Engn, Kowloon, Hong Kong 999077, Peoples R China;[4]East China Univ Sci & Technol, Sch Environm Sci & Engn, State Environm Protect Key Lab Environm Risk Asses, Shanghai 200237, Peoples R China;[5]Shanghai 4 Reagent Chem Co Ltd, Baoshan, Peoples R China

年份：2026

卷号：14

期号：1

外文期刊名：JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING

收录：;EI(收录号：20255219792988);WOS:【SCI-EXPANDED(收录号:WOS:001653520600009)】；

基金：This work was supported by the National Natural Science Foundation of China (NSFC) (22478119) and Xinjiang "Tianchi Talent" Project.

语种：英文

外文关键词：Electrocatalyst; Nitrate reduction; Copper; Ferric hydroxide; Ammonia desorption

摘要：Electrochemical reduction of nitrate (NO3-) to ammonia (NH3) represents a sustainable route for wastewater treatment and ammonia synthesis. Copper (Cu)-based catalysts, although effective for nitrate reduction, are limited by two major challenges: pronounced structural reconstruction and a strong tendency for ammonia adsorption, which causes active-site poisoning and rapid deactivation. To address these issues, we developed a Cu/Fe(OH)3 heterostructure catalyst using a facile controlled chemical deposition method. This composite architecture is designed to stabilize the active sites and mitigate NH3-induced poisoning, thereby enhancing both catalytic durability and performance. Density functional theory (DFT) calculations demonstrated that the hybridization between the d orbitals of Cu and Fe(OH)3 induced a downshift of the Cu D-band center from-2.079 eV to-2.086 eV, leading to a reduction in the adsorption energy barrier for reaction intermediates. Moreover, the DFT calculations indicated that the presence of Fe(OH)3 facilitated the adsorption of NO3-, while Cu promoted the desorption of NH3, collectively forming an efficient tandem electrocatalytic system. This synergistic tandem effect contributed to an exceptional nitrate reduction performance, achieving a current efficiency of 75.90 % and a high NH4+ selectivity of 98.22 % within 1 h of electrolysis, significantly outperforming both bare NF and Fe(OH)3/NF catalysts.