HFCAS OpenIR
Atomically dispersed bimetallic Fe-Co electrocatalysts for green production of ammonia
Zhang, Shengbo1,2; Han, Miaomiao3; Shi, Tongfei1,2; Zhang, Haimin1,2; Lin, Yue4; Zheng, Xusheng5; Zheng, Li Rong6; Zhou, Hongjian1,2; Chen, Chun1,2; Zhang, Yunxia1,2; Wang, Guozhong1,2; Yin, Huajie1,2; Zhao, Huijun7
2022-11-14
发表期刊NATURE SUSTAINABILITY
ISSN2398-9629
通讯作者Zhang, Haimin(zhanghm@issp.ac.cn) ; Zhao, Huijun(h.zhao@griffith.edu.au)
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.
DOI10.1038/s41893-022-00993-7
关键词[WOS]TOTAL-ENERGY CALCULATIONS ; ELECTROCHEMICAL SYNTHESIS ; NITROGEN ; CATALYST ; ELECTROREDUCTION ; EFFICIENCY ; CONVERSION ; REDUCTION ; WATER
收录类别SCI
语种英语
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
项目资助者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
WOS研究方向Science & Technology - Other Topics ; Environmental Sciences & Ecology
WOS类目Green & Sustainable Science & Technology ; Environmental Sciences ; Environmental Studies
WOS记录号WOS:000883302400002
出版者NATURE PORTFOLIO
引用统计
被引频次:29[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://ir.hfcas.ac.cn:8080/handle/334002/130324
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.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
2.Univ Sci & Technol China, Hefei, Peoples R China
3.Huzhou Univ, Sch Sci, Huzhou, Peoples R China
4.Univ Sci & Technol China, Hefei Natl Res Ctr Phys Sci Microscale, Hefei, Peoples R China
5.Univ Sci & Technol China, Natl Synchrotron Radiat Lab, Hefei, Peoples R China
6.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing, Peoples R China
7.Griffith Univ, Ctr Catalysis & Clean Energy, Gold Coast Campus, Southport, Qld, Australia
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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).
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