Atomically dispersed Au1 catalyst towards efficient electrochemical synthesis of ammonia

被引:237
|
作者
Wang, Xiaoqian [1 ]
Wang, Wenyu [1 ]
Qiao, Man [2 ]
Wu, Geng [1 ]
Chen, Wenxing [3 ,4 ]
Yuan, Tongwei [5 ]
Xu, Qian [6 ]
Chen, Min [1 ]
Zhang, Yan [1 ]
Wang, Xin [1 ]
Wang, Jing [1 ]
Ge, Jingjie [1 ]
Hong, Xun [1 ]
Li, Yafei [2 ]
Wu, Yuen [1 ]
Li, Yadong [3 ,4 ]
机构
[1] Univ Sci & Technol China, iChEM Collaborat Innovat Ctr Chem Energy Mat, Dept Chem, Hefei 230026, Anhui, Peoples R China
[2] Nanjing Normal Univ, Jiangsu Collaborat Innovat Ctr Biomed Funct Mat, Sch Chem & Mat Sci, Nanjing 210023, Jiangsu, Peoples R China
[3] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[4] Tsinghua Univ, Collaborat Innovat Ctr Nanomat Sci & Engn, Beijing 100084, Peoples R China
[5] Shanghai Univ, Coll Sci, Dept Chem, NEST Lab, Shanghai 200444, Peoples R China
[6] Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei 230029, Anhui, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
NH3; synthesis; Metal single sites; Electrocatalysis; Haber-Bosch process; Nitrogen reduction; TOTAL-ENERGY CALCULATIONS; OXYGEN REDUCTION; NITROGEN; WATER;
D O I
10.1016/j.scib.2018.07.005
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Tremendous efforts have been devoted to explore energy-efficient strategies of ammonia synthesis to replace Haber-Bosch process which accounts for 1.4% of the annual energy consumption. In this study, atomically dispersed Au-1 catalyst is synthesized and applied in electrochemical synthesis of ammonia under ambient conditions. A high NH4+ Faradaic efficiency of 11.1% achieved by our Au-1 catalyst surpasses most of reported catalysts under comparable conditions. Benefiting from efficient atom utilization, an NH4+ yield rate of 1,305 mu g h(-1) mg(Au)(1) has been reached, which is roughly 22.5 times as high as that by supported Au nanoparticles. We also demonstrate that by employing our Au-1 catalyst, NH4+ can be electro-chemically produced directly from N-2 and H-2 with an energy utilization rate of 4.02 mmol kJ(-1). Our study provides a possibility of replacing the Haber-Bosch process with environmentally benign and energy-efficient electrochemical strategies. (C) 2018 Science China Press. Published by Elsevier B.V. and Science China Press. All rights reserved.
引用
收藏
页码:1246 / 1253
页数:8
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