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题名: Photoprompted Hot Electrons from Bulk Cross-Linked Graphene Materials and Their Efficient Catalysis for Atmospheric Ammonia Synthesis
作者: Lu, Yanhong1, 2, 3, 5;  Yang, Yang1, 2, 3, 4;  Zhang, Tengfei1, 2, 3, 4;  Ge, Zhen1, 2, 3, 4;  Chang, Huicong1, 2, 3, 4;  Xiao, Peishuang1, 2, 3, 4;  Xie, Yuanyuan6;  Hua, Lei6;  Li, Qingyun6;  Li, Haiyang6;  Ma, Bo4;  Guan, Naijia4;  Ma, Yanfeng1, 2, 3, 4;  Chen, Yongsheng1, 2, 3, 4
关键词: graphene ;  photoprompted ;  hot electron ;  ammonia synthesis ;  atmospheric pressure
刊名: ACS NANO
发表日期: 2016-11-01
DOI: 10.1021/acsnano.6b06472
卷: 10, 期:11, 页:10507-10515
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences ;  Technology
类目[WOS]: Chemistry, Multidisciplinary ;  Chemistry, Physical ;  Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary
英文摘要: Ammonia synthesis is the single most important chemical process in industry and has used the successful heterogeneous Haber-Bosch catalyst for over 100 years and requires processing under both high temperature (300-500 degrees C) and pressure (200-300 atm); thus, it has huge energy costs accounting for about 1-3% of human's energy consumption. Therefore, there has been a long and vigorous exploration to find a milder alternative process. Here, we demonstrate that by using an iron- and graphene-based catalyst, Fe@3DGraphene, hot (ejected) electrons from this composite catalyst induced by visible light in a wide range of wavelength up to red could efficiently facilitate the activation of N-2 and generate ammonia with H-2 directly at ambient pressure using light (including simulated sun light) illumination directly. No external voltage or electrochemical or any other agent is needed. The production rate increases with increasing light frequency under the same power and with increasing power under the same frequency. The mechanism is confirmed by the detection of the intermediate N2H4 and also with a measured apparent activation energy only similar to 1/4 of the iron based Haber-Bosch catalyst. Combined with the morphology control using alumina as the structural promoter, the catalyst retains its activity in a 50 h test.
关键词[WOS]: NITROGENASE FEMO COFACTOR ;  SOLVATED ELECTRONS ;  CARRIER MULTIPLICATION ;  STABLE ELECTRIDE ;  REDUCTION ;  DINITROGEN ;  IRON ;  MECHANISM ;  PRESSURE ;  HYDROGEN
语种: 英语
WOS记录号: WOS:000388913100083
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/150348
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Nankai Univ, Ctr Nanoscale Sci & Technol, Tianjin 300071, Peoples R China
2.Nankai Univ, Key Lab Funct Polymer Mat, State Key Lab, Tianjin 300071, Peoples R China
3.Nankai Univ, Inst Elementoorgan Chem, Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Coll Chem, Tianjin 300071, Peoples R China
4.Nankai Univ, Sch Mat Sci & Engn, Natl Inst Adv Mat, Tianjin 300071, Peoples R China
5.Langfang Teachers Univ, Sch Chem & Mat Sci, Langfang 065000, Peoples R China
6.Chinese Acad Sci, Dalian Inst Chem Phys, Key Lab Separat Sci Analyt Chem, Dalian 116023, Peoples R China

Recommended Citation:
Lu, Yanhong,Yang, Yang,Zhang, Tengfei,et al. Photoprompted Hot Electrons from Bulk Cross-Linked Graphene Materials and Their Efficient Catalysis for Atmospheric Ammonia Synthesis[J]. ACS NANO,2016,10(11):10507-10515.
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