文献类型：期刊文献

英文题名：High-Loading Cu Single-Atom Engineering on g-C3N4 for Visible-Light CO2 Photoreduction

作者：Wang, Lijie[1,2];Li, Jiaying[1,2];Zhong, Chenggui[1,2];He, Chengxuan[1,2];Khan, Mazhar[1,2];Liu, Dongni[1,2];Wang, Jinlong[1,2];Yang, Ruijie[1,2];Kan, Miao[1,2];Wang, Lingzhi[1,2];Wu, Shiqun[1,2];Zhang, Jinlong[1,2]

机构：[1]East China Univ Sci & Technol, State Key Lab Green Chem Engn & Ind Catalysis, Key Lab Adv Mat & Joint Int Res Lab Precis Chem &, Feringa Nobel Prize Scientist Joint Res Ctr,Sch Ch, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Shanghai Engn Res Ctr Multimedia Environm Catalysi, Shanghai 200237, Peoples R China

年份：2025

卷号：21

期号：27

外文期刊名：SMALL

收录：;WOS:【SCI-EXPANDED(收录号:WOS:001489576700001)】；

基金：This work was supported by National Key Research and Development Program of China (2022YFE0107900, 2022YFB3803600), the National Natural Science Foundation of China (22202070, 22461142136), the Innovation Program of Shanghai Municipal Education Commission (2021-01-07-00-02-E00106), the Science and Technology Commission of Shanghai Municipality (22230780200, 20DZ2250400, 2018SHZDZX03), the Chenguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission (24CGA30), the Shanghai Rising-Star Program (22YF1410200), and Fundamental Research Funds for the Central Universities (222201717003).

语种：英文

外文关键词：CO2 photoreduction; Cu single atom; g-C3N4; high loading

摘要：The incorporation of metal single atoms into carbon nitride (CN) has emerged as a promising strategy for photocatalytic CO2 reduction under visible light. However, achieving high single-atom loading and unraveling the precise role of active metal centers in CO2 conversion remain formidable challenges. Herein, an ultrasound-assisted coordination exchange strategy is reported that enables the high-loading of Cu single atoms on CN. X-ray absorption near-edge spectroscopy and aberration-corrected electron microscopy confirm that Cu is atomically dispersed and coordinated with nitrogen. The introduction of Cu single atoms modulates the electronic structure of CN, serving as electron accumulation centers that facilitate charge carrier separation and transfer. Theoretical calculations combined with in situ spectroscopic analyses reveal that Cu single atoms act as active sites, enhancing CO2 adsorption and activation while significantly reducing the energy barrier for *COOH formation, thereby optimizing reaction thermodynamics. As a result, under visible-light irradiation, Cu-modified CN achieves a CO production rate of 14.65 mu mol g(-)(1) h(-)(1), representing an 11.3-fold enhancement over pristine CN. This work not only establishes an efficient approach for synthesizing high-loading single-atom catalysts but also provides fundamental insights into the mechanistic role of single-atom sites in photocatalytic CO2 reduction.