Unveiling the size effect of nitrogen-doped carbon-supported copper-based catalysts on nitrate-to-ammonia electroreduction

作     者：Ran Li Taotao Gao Wenxi Qiu Minghao Xie Zhaoyu Jin Panpan Li Ran Li;Taotao Gao;Wenxi Qiu;Minghao Xie;Zhaoyu Jin;Panpan Li

作者机构：College of Materials Science and EngineeringSichuan UniversityChengdu 610065China Institute for Advanced StudyChengdu UniversityChengdu 610106China Materials Science and Engineering Program and Walker Department of Mechanical EngineeringThe University of Texas at AustinAustinTexas 78712USA Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 610054China 

出 版 物：《Nano Research》 (纳米研究（英文版）)

年 卷 期：2024年第17卷第4期

页      面：2438-2443页

核心收录：

学科分类：081704[工学-应用化学] 07[理学] 070304[理学-物理化学(含∶化学物理)] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 0703[理学-化学] 0702[理学-物理学] 

基　　金：support from the National Nature Science Foundation of China(No.52202372) the Sichuan Science and Technology Program(Nos.2023NSFSC0436 and 2023NSFSC0089) the Fundamental Research Funds for the Central Universities(Nos.YJ2021151 and 20826041G4185) T.T.G.acknowledges the Chengdu University new faculty start-up funding(No.2081920074) 

主　　题：nitrate electroreduction ammonia electrosynthesis size effect single-cluster catalyst 

摘      要：The electrocatalytic nitrate reduction reaction(NitRR)represents a promising approach toward achieving economically and environmentally sustainable ***,it remains a challenge to regulate the size effect of electrocatalysts to optimize the catalytic activity and ammonia ***,the Cu-based catalysts were tailored at the atomic level to exhibit a size gradient ranging from single-atom catalysts(SACs,0.15–0.35 nm)to single-cluster catalysts(SCCs,1.0–2.8 nm)and nanoparticles(NPs,20–30 nm),with the aim of studying the size effect for the NO_(3)^(-)-to-NH_(3) reduction ***,the Cu SCCs exhibit enhanced metal–substrate and metal–metal interactions by taking advantageous features of Cu SACs and Cu ***,Cu SCCs achieve exceptional electrocatalytic performance for the NitRR with a maximum Faradaic efficiency of ca.96%NH_(3)and the largest yield rate of ca.1.99 mg·h^(-1)·cm^(-2) at-0.5 V *** hydrogen electrode(RHE).The theoretical calculation further reveals the size effect and coordination environment on the high catalytic activity and selectivity for the *** work provides a promising various size-controlled design strategy for aerogel-based catalysts effectively applied in various electrocatalytic reactions.