Self-Triggering a Locally Alkaline Microenvironment of Co4Fe6 for Highly Efficient Neutral Ammonia Electrosynthesis
文献类型：期刊论文
| 作者 | Yang, Yang1,2; Sun, Yuting1,3; Wang, Yuning1,4; Zhang, Xiaoxue5; Zhang, Wenyu1,2; Huang, Zhen-Feng5; Yin, Lichang1,2; Han, Ali1; Liu, Gang1,2 |
| 刊名 | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
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| 出版日期 | 2025-02-28 |
| 卷号 | 147期号:10页码:8893-8905 |
| ISSN号 | 0002-7863 |
| DOI | 10.1021/jacs.5c00688 |
| 通讯作者 | Han, Ali(alhan@imr.ac.cn) ; Liu, Gang(gangliu@imr.ac.cn) |
| 英文摘要 | 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 |
| 语种 | 英语 |
| WOS记录号 | WOS:001435214100001 |
| 出版者 | AMER CHEMICAL SOC |
| 资助机构 | National Natural Science Foundation of China ; National Natural Science Foundation of China ; New Cornerstone Science Foundation through the XPLORER PRIZE |
| 源URL |  |
| 专题 | 金属研究所_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. |
入库方式： OAI收割
来源：金属研究所
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