文献类型：期刊文献

英文题名：High-Loading Cu Single-Atom Engineering on g-C?N? for Visible-Light CO? 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] State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering, Feringa Nobel Prize Scientist Joint Research Center, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, China; [2] Shanghai Engineering Research Center for Multi-media Environmental Catalysis and Resource Utilization, East China University of Science and Technology, Shanghai, 200237, China

年份：2025

卷号：21

期号：27

外文期刊名：Small

收录：EI(收录号：20252118447628)

语种：英文

外文关键词：Diffusion

摘要：The incorporation of metal single atoms into carbon nitride (CN) has emerged as a promising strategy for photocatalytic CO? reduction under visible light. However, achieving high single-atom loading and unraveling the precise role of active metal centers in CO? 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 CO? 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 14.65μmol 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 CO? reduction. ? 2025 Wiley-VCH GmbH.