Highly Productive Electrosynthesis of Ammonia by Admolecule-Targeting Single Ag Sites

doi:10.1021/acsnano.0c01340

CORC > 兰州理工大学 > 兰州理工大学 > 省部共建有色金属先进加工与再利用国家重点实验室

	Highly Productive Electrosynthesis of Ammonia by Admolecule-Targeting Single Ag Sites
	Chen, Ying 3; Guo, Ruijie 3; Peng, Xianyun 3; Wang, Xiaoqian 2; Liu, Xijun 3; Ren, Junqiang 1; He, Jia 3; Zhuo, Longchao 5; Sun, Jiaqiang 4; Liu, Yifan 6
刊名	ACS Nano
	2020-06-23
卷号	14 期号:6 页码:6938-6946
关键词	Ammonia Calculations Chlorine compounds Electrocatalysts Ambient conditions Consecutive reaction Design Principles Faradaic efficiencies First-principles calculation Haber-Bosch process Reduction current Reduction reaction
ISSN号	19360851
DOI	10.1021/acsnano.0c01340
英文摘要	The ambient electrocatalytic N2 reduction reaction (NRR) is a promising alternative to the Haber-Bosch process for producing NH3. However, a guideless search for single-atom-based and other electrocatalysts cannot promote the NH3 yield rates by NRR efficiently. Herein, our first-principles calculations reveal that the successive emergence of vertical end-on N2 and oblique end-on NNH admolecules on single metal sites is key to high-performance NRR. By targeting the admolecules, single Ag sites with the Ag-N4 coordination are found and synthesized massively. They exhibit a record-high NH3 yield rate (270.9 μg h-1 mgcat.-1 or 69.4 mg h-1 mgAg-1) and a desirable Faradaic efficiency (21.9%) in HCl aqueous solution under ambient conditions. The generation rate of NH3 is stable during 20 consecutive reaction cycles, and the reduction current density is almost constant for 60 h. This work provides an effective targeting-design principle to purposefully synthesize active and durable single-atom-based NRR electrocatalysts. © 2020 American Chemical Society.
WOS研究方向	Chemistry ; Science & Technology - Other Topics ; Materials Science
语种	英语
出版者	American Chemical Society
WOS记录号	WOS:000543744100053
内容类型	期刊论文
源URL	[http://ir.lut.edu.cn/handle/2XXMBERH/151176]
专题	省部共建有色金属先进加工与再利用国家重点实验室继续教育学院
作者单位	1.State Key Laboratory of Advanced Processing and Recycling of Nonferrous Metals, Lanzhou University of Technology, Lanzhou; 730050, China; 2.School of Chemistry and Materials Science, IChEM, CAS Center for Excellence in Nanoscience, University of Science and Technology of China, Hefei National Laboratory for Physical Sciences at the Microscale, Hefei; 230026, China; 3.Center for Electron Microscopy, Tianjin Key Lab of Advanced Functional Porous Materials, Institute for New Energy Materials and Low-Carbon Technologies, School of Materials Science and Engineering, Tianjin University of Technology, Tianjin; 300384, China; 4.State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan; 030001, China; 5.School of Materials Science and Engineering, Xi'An University of Technology, Xi'an; 710048, China; 6.College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen; 518060, China
推荐引用方式 GB/T 7714	Chen, Ying,Guo, Ruijie,Peng, Xianyun,et al. Highly Productive Electrosynthesis of Ammonia by Admolecule-Targeting Single Ag Sites[J]. ACS Nano,2020,14(6):6938-6946.
APA	Chen, Ying.,Guo, Ruijie.,Peng, Xianyun.,Wang, Xiaoqian.,Liu, Xijun.,...&Luo, Jun.(2020).Highly Productive Electrosynthesis of Ammonia by Admolecule-Targeting Single Ag Sites.ACS Nano,14(6),6938-6946.
MLA	Chen, Ying,et al."Highly Productive Electrosynthesis of Ammonia by Admolecule-Targeting Single Ag Sites".ACS Nano 14.6(2020):6938-6946.