{"title":"以Co为活性中心的FeCo双原子催化剂在酸性氧还原反应中的双面效应","authors":"Long-Ji Yuan, Zhen-Yu Miao, Xu-Lei Sui, Chi-Feng Lee, Qi Li, Mei-Jie Yin, Li-Xiao Shen, Ying-Rui Lu, Zi-Gang Zhao, Yu-Zhe Liu, Lin-Sheng Zhu, Wei Gong, Wen-Liang Feng, Hsiao-Tsu Wang, Guo-Xu Zhang, Zhen-Bo Wang","doi":"10.1038/s41467-025-62728-4","DOIUrl":null,"url":null,"abstract":"<p>Dual-atom catalysts (DACs) represent a frontier in heterogeneous electrocatalysis for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. However, the dynamic evolution of active-site structure complicates mechanistic understanding. Herein, alloyed Fe-Co DACs with strong Fe-Co bonds are synthesized via molecular chelation and ionic coupling strategies. In-situ spectroscopy combined with theoretical calculation reveals the Janus effect of Fe-Co dual-atom sites: Co serves as the primary catalytic center for the 4e<sup>-</sup> process with Fe as the cooperative sites to absorb the *OH. This division-of-labor mechanism lowers the theoretical overpotential from 1.14 V to 0.43 V for acidic oxygen reduction reaction. Thus, the catalyst achieves a 0.852 V half-wave potential and 1.14 W cm<sup>−2</sup> power density (2.0 bar H₂-O₂), sustaining 81% peak power after 10,000 cycles. These findings clarify DAC configuration-mechanism relationships, guiding the design of high-performance DACs.</p>","PeriodicalId":19066,"journal":{"name":"Nature Communications","volume":"13 1","pages":""},"PeriodicalIF":15.7000,"publicationDate":"2025-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Janus effect of FeCo dual atom catalyst with Co as active center in acidic oxygen reduction reaction\",\"authors\":\"Long-Ji Yuan, Zhen-Yu Miao, Xu-Lei Sui, Chi-Feng Lee, Qi Li, Mei-Jie Yin, Li-Xiao Shen, Ying-Rui Lu, Zi-Gang Zhao, Yu-Zhe Liu, Lin-Sheng Zhu, Wei Gong, Wen-Liang Feng, Hsiao-Tsu Wang, Guo-Xu Zhang, Zhen-Bo Wang\",\"doi\":\"10.1038/s41467-025-62728-4\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Dual-atom catalysts (DACs) represent a frontier in heterogeneous electrocatalysis for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. However, the dynamic evolution of active-site structure complicates mechanistic understanding. Herein, alloyed Fe-Co DACs with strong Fe-Co bonds are synthesized via molecular chelation and ionic coupling strategies. In-situ spectroscopy combined with theoretical calculation reveals the Janus effect of Fe-Co dual-atom sites: Co serves as the primary catalytic center for the 4e<sup>-</sup> process with Fe as the cooperative sites to absorb the *OH. This division-of-labor mechanism lowers the theoretical overpotential from 1.14 V to 0.43 V for acidic oxygen reduction reaction. Thus, the catalyst achieves a 0.852 V half-wave potential and 1.14 W cm<sup>−2</sup> power density (2.0 bar H₂-O₂), sustaining 81% peak power after 10,000 cycles. These findings clarify DAC configuration-mechanism relationships, guiding the design of high-performance DACs.</p>\",\"PeriodicalId\":19066,\"journal\":{\"name\":\"Nature Communications\",\"volume\":\"13 1\",\"pages\":\"\"},\"PeriodicalIF\":15.7000,\"publicationDate\":\"2025-08-05\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Communications\",\"FirstCategoryId\":\"103\",\"ListUrlMain\":\"https://doi.org/10.1038/s41467-025-62728-4\",\"RegionNum\":1,\"RegionCategory\":\"综合性期刊\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"MULTIDISCIPLINARY SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Communications","FirstCategoryId":"103","ListUrlMain":"https://doi.org/10.1038/s41467-025-62728-4","RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"MULTIDISCIPLINARY SCIENCES","Score":null,"Total":0}
引用次数: 0
摘要
双原子催化剂是质子交换膜燃料电池氧还原反应多相电催化研究的前沿。然而,活性位点结构的动态演变使机理理解复杂化。本文通过分子螯合和离子偶联策略合成了具有强Fe-Co键的Fe-Co合金dac。原位光谱结合理论计算揭示了Fe-Co双原子位的Janus效应:Co作为4e-过程的一级催化中心,Fe作为吸附*OH的辅助位。这种分工机制使酸性氧还原反应的理论过电位从1.14 V降低到0.43 V。因此,催化剂达到了0.852 V的半波电位和1.14 W cm−2的功率密度(2.0 bar H₂-O₂),在10,000次循环后保持81%的峰值功率。这些发现阐明了DAC配置与机制的关系,对高性能DAC的设计具有指导意义。
Janus effect of FeCo dual atom catalyst with Co as active center in acidic oxygen reduction reaction
Dual-atom catalysts (DACs) represent a frontier in heterogeneous electrocatalysis for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells. However, the dynamic evolution of active-site structure complicates mechanistic understanding. Herein, alloyed Fe-Co DACs with strong Fe-Co bonds are synthesized via molecular chelation and ionic coupling strategies. In-situ spectroscopy combined with theoretical calculation reveals the Janus effect of Fe-Co dual-atom sites: Co serves as the primary catalytic center for the 4e- process with Fe as the cooperative sites to absorb the *OH. This division-of-labor mechanism lowers the theoretical overpotential from 1.14 V to 0.43 V for acidic oxygen reduction reaction. Thus, the catalyst achieves a 0.852 V half-wave potential and 1.14 W cm−2 power density (2.0 bar H₂-O₂), sustaining 81% peak power after 10,000 cycles. These findings clarify DAC configuration-mechanism relationships, guiding the design of high-performance DACs.
期刊介绍:
Nature Communications, an open-access journal, publishes high-quality research spanning all areas of the natural sciences. Papers featured in the journal showcase significant advances relevant to specialists in each respective field. With a 2-year impact factor of 16.6 (2022) and a median time of 8 days from submission to the first editorial decision, Nature Communications is committed to rapid dissemination of research findings. As a multidisciplinary journal, it welcomes contributions from biological, health, physical, chemical, Earth, social, mathematical, applied, and engineering sciences, aiming to highlight important breakthroughs within each domain.