Self-Triggering a Locally Alkaline Microenvironment of Co<sub>4</sub>Fe<sub>6</sub> for Highly Efficient Neutral Ammonia Electrosynthesis

doi:10.1021/jacs.5c00688

IMR OpenIR

	Self-Triggering a Locally Alkaline Microenvironment of Co₄Fe₆ for Highly Efficient Neutral Ammonia Electrosynthesis
	Yang, Yang 1,2; Sun, Yuting 1,3; Wang, Yuning 1,4; Zhang, Xiaoxue 5; Zhang, Wenyu 1,2; Huang, Zhen-Feng 5; Yin, Lichang 1,2; Han, Ali 1; Liu, Gang 1,2
通讯作者	Han, Ali(alhan@imr.ac.cn) ; Liu, Gang(gangliu@imr.ac.cn)
	2025-02-28
发表期刊	JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
ISSN	0002-7863
卷号	147 期号:10 页码:8893-8905
摘要	Electrochemical nitrate reduction reaction (eNO3 -RR) to ammonia (NH3) holds great promise for the green treatment of NO3 - and ambient NH3 synthesis. Although Fe-based electrocatalysts have emerged as promising alternatives, their excellent eNO3 -RR-to-NH3 activity is usually limited to harsh alkaline electrolytes or alloying noble metals with Fe in sustainable neutral electrolytes. Herein, we demonstrate an unusual self-triggering localized alkalinity of the Co4Fe6 electrocatalyst for efficient eNO3 -RR-to-NH3 activity in neutral media, which breaks down the conventional pH-dependent kinetics restrictions and shows a 98.6% NH3 Faradaic efficiency (FE) and 99.9% NH3 selectivity at -0.69 V vs RHE. The synergetic Co-Fe dual sites were demonstrated to enable the optimal free energies of eNO3 -RR-to-NH3 species and balance water dissociation and protonation of adsorbed NO2 -. Notably, the Co4Fe6 electrocatalysts can attain a high current density of 100 mA cm-2 with a high NH3 FE surpassing 96% and long-term stability for over 500 h eNO3 -RR-to-NH3 in a membrane electrode assembly (MEA) electrolyzer. This work provides insight into tailoring the self-reinforced local-alkalinity on the Fe-based alloy electrocatalysts for eNO3 -RR-to-NH3 and thus avoids alkaline electrolytes and noble metals for practical sustainable nitrate upcycling technology.
资助者	National Natural Science Foundation of China ; National Natural Science Foundation of China ; New Cornerstone Science Foundation through the XPLORER PRIZE
DOI	10.1021/jacs.5c00688
收录类别	SCI
语种	英语
资助项目	National Natural Science Foundation of China[52425201] ; National Natural Science Foundation of China[22202214] ; National Natural Science Foundation of China ; New Cornerstone Science Foundation through the XPLORER PRIZE
WOS研究方向	Chemistry
WOS类目	Chemistry, Multidisciplinary
WOS记录号	WOS:001435214100001
出版者	AMER CHEMICAL SOC
引用统计
文献类型	期刊论文
条目标识符	http://ir.imr.ac.cn/handle/321006/179791
专题	中国科学院金属研究所
通讯作者	Han, Ali; Liu, Gang
作者单位	1.Chinese Acad Sci, Inst Met Res, Shenyang Natl Lab Mat Sci, Shenyang 110016, Peoples R China 2.Univ Sci & Technol China, Sch Mat Sci & Engn, Shenyang 110016, Peoples R China 3.Dalian Univ Technol, Engn Res Ctr High Entropy Alloy Mat Liaoning Prov, Sch Mat Sci & Engn, Dalian 116024, Peoples R China 4.Northeastern Univ, Sch Mat Sci & Engn, Shenyang 110819, Liaoning, Peoples R China 5.Tianjin Univ, Sch Chem Engn & Technol, Tianjin 300072, Peoples R China
推荐引用方式 GB/T 7714	Yang, Yang,Sun, Yuting,Wang, Yuning,et al. Self-Triggering a Locally Alkaline Microenvironment of Co₄Fe₆ for Highly Efficient Neutral Ammonia Electrosynthesis[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2025,147(10):8893-8905.
APA	Yang, Yang.,Sun, Yuting.,Wang, Yuning.,Zhang, Xiaoxue.,Zhang, Wenyu.,...&Liu, Gang.(2025).Self-Triggering a Locally Alkaline Microenvironment of Co₄Fe₆ for Highly Efficient Neutral Ammonia Electrosynthesis.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,147(10),8893-8905.
MLA	Yang, Yang,et al."Self-Triggering a Locally Alkaline Microenvironment of Co₄Fe₆ for Highly Efficient Neutral Ammonia Electrosynthesis".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147.10(2025):8893-8905.