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Single atom accelerates ammonia photosynthesis

文献类型：期刊论文

作者Huang, Pengcheng1; Liu, Wei2; He, Zhihai1; Xiao, Chong1; Yao, Tao2; Zou, Youming3; Wang, Chengming1; Qi, Zeming2; Tong, Wei3; Pan, Bicai1
刊名SCIENCE CHINA-CHEMISTRY
出版日期2018-09-01
卷号61期号:9页码:1187-1196
关键词single atom photocatalytic ammonia synthesis
ISSN号1674-7291
DOI10.1007/s11426-018-9273-1
通讯作者Xiao, Chong(cxiao@ustc.edu.cn) ; Xie, Yi(yxie@ustc.edu.cn)
英文摘要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 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 NH3 producing rate of copper modified carbon nitride (Cu-CN) reached 186 mol 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.
WOS关键词GRAPHITIC CARBON NITRIDE ; AUGMENTED-WAVE METHOD ; HYDROGEN EVOLUTION ; HETEROGENEOUS CATALYSIS ; NITROGEN-FIXATION ; PHOTOCATALYSTS ; REDUCTION ; WATER ; ACTIVATION ; NANOSHEETS
资助项目National Key R&D Program of China[2017YFA0207301] ; National Natural Science Foundation of China[21622107] ; National Natural Science Foundation of China[11621063] ; National Natural Science Foundation of China[U1532265] ; Key Research Program of Frontier Sciences[QYZDY-SSW-SLH011] ; Youth Innovation Promotion Association CAS[2016392] ; Fundamental Research Funds of Central University[WK2340000075] ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology[2017FXZY003]
WOS研究方向Chemistry
语种英语
WOS记录号WOS:000447772000017
出版者SCIENCE PRESS
资助机构National Key R&D Program of China ; National Key R&D Program of China ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; National Key R&D Program of China ; National Key R&D Program of China ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; National Key R&D Program of China ; National Key R&D Program of China ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; National Key R&D Program of China ; National Key R&D Program of China ; National Key R&D Program of China ; National Key R&D Program of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Key Research Program of Frontier Sciences ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Youth Innovation Promotion Association CAS ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Fundamental Research Funds of Central University ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology ; Major Program of Development Foundation of Hefei Center for Physical Science and Technology
源URL[http://ir.hfcas.ac.cn:8080/handle/334002/39714]  
专题合肥物质科学研究院_中科院强磁场科学中心
通讯作者Xiao, Chong; Xie, Yi
作者单位1.Univ Sci & Technol China, CAS Ctr Excellence Nanosci, iCHEM, Hefei Natl Lab Phys Sci Microscale, Hefei 230026, Anhui, Peoples R China
2.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China
3.Chinese Acad Sci, High Field Magnet Lab, Hefei 230031, Anhui, Peoples R China
推荐引用方式
GB/T 7714		 Huang, Pengcheng,Liu, Wei,He, Zhihai,et al. Single atom accelerates ammonia photosynthesis[J]. SCIENCE CHINA-CHEMISTRY,2018,61(9):1187-1196.
APA Huang, Pengcheng.,Liu, Wei.,He, Zhihai.,Xiao, Chong.,Yao, Tao.,...&Xie, Yi.(2018).Single atom accelerates ammonia photosynthesis.SCIENCE CHINA-CHEMISTRY,61(9),1187-1196.
MLA Huang, Pengcheng,et al."Single atom accelerates ammonia photosynthesis".SCIENCE CHINA-CHEMISTRY 61.9(2018):1187-1196.

入库方式： OAI收割

来源：合肥物质科学研究院

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