Single atom accelerates ammonia photosynthesis

作     者：Pengcheng Huang Wei Liu Zhihai He Chong Xiao Tao Yao Youming Zou Chengming Wang Zeming Qi Wei Tong Bicai Pan Shiqiang Wei Yi Xie 

作者机构：Hefet National Laboratory for Physical Sciences at the Microscale CAS Center for Excellence in Nanoscience iCHEM University of Science and Technology of China Hefei 230026 China National Synchrotron Radiation Laboratory University of Science and Technology of China. Hefei 230029 China High Magnetic Field Laboratory Chinese Academy of Sciences Hefei 230031 China 

出 版 物：《Science China Chemistry》 (中国科学（化学英文版）)

年 卷 期：2018年第61卷第9期

页      面：1187-1196页

核心收录：

学科分类：081702[工学-化学工艺] 08[工学] 0817[工学-化学工程与技术] 

基　　金：supported by the National Key R&D Program of China (2017YFA0207301) the National Natural Science Foundation of China (21622107, 11621063, U1532265) the Key Research Program of Frontier Sciences (QYZDY-SSW-SLH011), the Youth Innovation Promotion Association CAS (2016392) the Fundamental Research Funds of Central University (WK2340000075) the Major Program of Development Foundation of Hefei Center for Physical Science and Technology (2017FXZY003) 

主　　题：single atom photocatalytic ammonia synthesis 

摘      要：Atomically dispersed metal has gained much attention because of the new opportunities they offer in catalysis. However, it is still crucial to understand the mechanism of single-atom catalysis at molecular level for expanding them to other more difficult catalytic reactions, such as ammonia synthesis from nitrogen. In fact, developing ammonia synthesis under ambient conditions to overcome the high energy consumption in well-established Haber-Bosch process has fascinated scientists for many ***, we demonstrate that single Cu atom yields facile valence-electron isolation from the conjugated π electron cloud of p-CN. Electron spin resonance measurements reveal that these isolated valence electrons can be easily excited to generate free electrons under photo-illumination, thus inducing high efficient photo-induced ammonia synthesis under ambient *** NH_3 producing rate of copper modified carbon nitride(Cu-CN) reached 186 μmol g^(-1) h^(-1) under visible light irradiation with the quantum efficiency achieved 1.01% at 420 nm monochromatic light. This finding surely offers a model to open up a new vista for the ammonia synthesis at gentle conditions. The introduction of single atom to isolate the valence electron also represents a new paradigm for many other photocatalytic reactions, since the most photoinduced processes have been successfully exploited sharing the same origin.