Atomically dispersed bimetallic Fe-Co electrocatalysts for green production of ammonia

doi:10.1038/s41893-022-00993-7

	Atomically dispersed bimetallic Fe-Co electrocatalysts for green production of ammonia
	Zhang, Shengbo 1,6; Han, Miaomiao 7; Shi, Tongfei 1,6; Zhang, Haimin 1,6; Lin, Yue 2; Zheng, Xusheng 5; Zheng, Li Rong 4; Zhou, Hongjian 1,6; Chen, Chun 1,6; Zhang, Yunxia 1,6
刊名	NATURE SUSTAINABILITY
	2022-11-14
ISSN号	2398-9629
DOI	10.1038/s41893-022-00993-7
通讯作者	Zhang, Haimin(zhanghm@issp.ac.cn) ; Zhao, Huijun(h.zhao@griffith.edu.au)
英文摘要	The dominant Haber-Bosch process to produce ammonia, arguably the most important chemical in support of global food supply, is both energy and carbon intensive, resulting in substantial environmental impacts. Electrocatalytic nitrogen reduction reaction (NRR) powered by renewable electricity provides a green synthetic route for ammonia, but still suffers from insufficient yield rate and Faradaic efficiency. Single-atom electrocatalysts (SACs) have the potential to transform this catalytic process; however, controllable synthesis of SACs with high loading of active sites remains a big challenge. Here we utilize bacterial cellulose with rich oxygen functional groups to anchor iron (Fe) and cobalt (Co), realizing high density, atomically dispersed, bimetallic Fe-Co active sites. For electrocatalytic NRR, our catalyst design delivers a remarkable ammonia yield rate of 579.2 +/- 27.8 mu g h(-1) mg(cat.)(-1) and an exceptional Faradaic efficiency of 79.0 +/- 3.8%. The combined theoretical and experimental investigations reveal that the operando change in coordination configuration from [(O-C-2)(3)Fe-Co(O-C-2)(3)] to [(O-C-2)(3)Fe-Co(O-C)C-2] is the enabling chemistry. Our findings suggest a general approach to engineer SACs that can drive critical reactions of relevance for sustainability. Electrocatalytic reduction of nitrogen has emerged as a sustainable means for the production of ammonia. Here the authors design bimetallic Fe-Co single-atom catalysts dispersed on carbon that enable unprecedented ammonia yield rates.
资助项目	Natural Science Foundation of China[52172106] ; Natural Science Foundation of China[51872292] ; Natural Science Foundation of China[61804154] ; Natural Science Foundation of China[52122212] ; Youth Innovation Promotion Association of the CAS[2020458] ; National Key Research and Development Program of China[2019YFA0307900] ; Anhui Provincial Natural Science Foundation[2108085QB60] ; CASHIPS Director's Fund[YZJJ2021QN18] ; China Postdoctoral Science Foundation[2020M682057] ; Special Research Assistant Program, Chinese Academy of Sciences ; CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China ; Beijing Synchrotron Radiation Facility
WOS关键词	TOTAL-ENERGY CALCULATIONS ; ELECTROCHEMICAL SYNTHESIS ; NITROGEN ; CATALYST ; ELECTROREDUCTION ; EFFICIENCY ; CONVERSION ; REDUCTION ; WATER
WOS研究方向	Science & Technology - Other Topics ; Environmental Sciences & Ecology
语种	英语
出版者	NATURE PORTFOLIO
WOS记录号	WOS:000883302400002
资助机构	Natural Science Foundation of China ; Youth Innovation Promotion Association of the CAS ; National Key Research and Development Program of China ; Anhui Provincial Natural Science Foundation ; CASHIPS Director's Fund ; China Postdoctoral Science Foundation ; Special Research Assistant Program, Chinese Academy of Sciences ; CAS/SAFEA International Partnership Program for Creative Research Teams of Chinese Academy of Sciences, China ; Beijing Synchrotron Radiation Facility
内容类型	期刊论文
源URL	[http://ir.hfcas.ac.cn:8080/handle/334002/130323]
专题	中国科学院合肥物质科学研究院
通讯作者	Zhang, Haimin; Zhao, Huijun
作者单位	1.Univ Sci & Technol China, Hefei, Peoples R China 2.Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Hefei, Peoples R China 3.Griffith Univ, Ctr Catalysis & Clean Energy, Gold Coast Campus, Southport, Qld, Australia 4.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing, Peoples R China 5.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei, Peoples R China 6.Chinese Acad Sci, Ctr Environm & Energy Nanomat, CAS Ctr Excellence Nanosci,HFIPS, Inst Solid State Phys,Key Lab Mat Phys,Anhui Key, Hefei, Peoples R China 7.Huzhou Univ, Sch Sci, Huzhou, Peoples R China
推荐引用方式 GB/T 7714	Zhang, Shengbo,Han, Miaomiao,Shi, Tongfei,et al. Atomically dispersed bimetallic Fe-Co electrocatalysts for green production of ammonia[J]. NATURE SUSTAINABILITY,2022.
APA	Zhang, Shengbo.,Han, Miaomiao.,Shi, Tongfei.,Zhang, Haimin.,Lin, Yue.,...&Zhao, Huijun.(2022).Atomically dispersed bimetallic Fe-Co electrocatalysts for green production of ammonia.NATURE SUSTAINABILITY.
MLA	Zhang, Shengbo,et al."Atomically dispersed bimetallic Fe-Co electrocatalysts for green production of ammonia".NATURE SUSTAINABILITY (2022).