Single atom accelerates ammonia photosynthesis

查看全文 作　　者：Pengcheng [1]Huang;Wei [2]Liu;Zhihai [1]He;Chong [1]Xiao;Tao [2]Yao;Youming [3]Zou;Chengming [1]Wang;Zeming [2]Qi;Wei [3]Tong;Bicai [1]Pan;Shiqiang [2]Wei;Yi [1]Xie

机构地区：[1]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;[2]National Synchrotron Radiation Laboratory, University of Science and Technology of China. Hefei 230029, China;[3]High Magnetic Field Laboratory, Chinese Academy of Sciences, Hefei 230031, China

出　　处：《Science China Chemistry》索引2018年第61卷第9期,共10页

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) 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 years.Herein, 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 conditions.The 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. 关键词：氨合成原子光合作用催化作用催化反应碳氮化物价电子科学家

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Single atom accelerates ammonia photosynthesis

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