Furi Wang, Xujiao Ma, Xiaofang Su, Zhong Zhang, Wei Liu, Jiahui Peng, Zongyin Gao, Jian Zhang, Yiwei Liu
{"title":"Efficient Oxygen Reduction Catalysis on Fe4 Cluster Site Facilitated by Adjacent Single Atom","authors":"Furi Wang, Xujiao Ma, Xiaofang Su, Zhong Zhang, Wei Liu, Jiahui Peng, Zongyin Gao, Jian Zhang, Yiwei Liu","doi":"10.1002/smll.202501746","DOIUrl":null,"url":null,"abstract":"The inherent sluggish kinetics of the conventional four-electron transfer pathway fundamentally limits the oxygen reduction reaction (ORR) efficiency. While electronic structure modulation offers potential solutions, developing effective catalytic regulation strategies remains challenging due to elusive structure-activity correlations. In this study, Fe<sub>4</sub> cluster sites are engineered with dual parallel electron transfer channels that enable concurrent O─O bond cleavage and dual oxygen atom protonation. This unique configuration facilitates an optimized two-step double electron transfer mechanism, significantly enhancing ORR kinetics. Synergistic Mn single atom sites, strategically positioned as electron reservoirs, substantially elevate the electron density of Fe<sub>4</sub> clusters while reinforcing Fe─N coordination bonds through charge redistribution. Remarkably, the spatial configuration of Fe<sub>4</sub> clusters at the support periphery minimizes steric confinement effects, allowing simultaneous product desorption and oxygen adsorption – a critical advantage for sustaining continuous catalytic cycles. Through combined experimental and theoretical analyses, it is demonstrated that this dual-channel electron transport system effectively reduces activation barriers for elementary steps while accelerating charge transfer kinetics. This fundamental study establishes a new paradigm for designing high-performance ORR catalysts through multi-site collaborative engineering and reaction pathway optimization.","PeriodicalId":228,"journal":{"name":"Small","volume":"27 1","pages":""},"PeriodicalIF":13.0000,"publicationDate":"2025-03-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Small","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1002/smll.202501746","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
Abstract
The inherent sluggish kinetics of the conventional four-electron transfer pathway fundamentally limits the oxygen reduction reaction (ORR) efficiency. While electronic structure modulation offers potential solutions, developing effective catalytic regulation strategies remains challenging due to elusive structure-activity correlations. In this study, Fe4 cluster sites are engineered with dual parallel electron transfer channels that enable concurrent O─O bond cleavage and dual oxygen atom protonation. This unique configuration facilitates an optimized two-step double electron transfer mechanism, significantly enhancing ORR kinetics. Synergistic Mn single atom sites, strategically positioned as electron reservoirs, substantially elevate the electron density of Fe4 clusters while reinforcing Fe─N coordination bonds through charge redistribution. Remarkably, the spatial configuration of Fe4 clusters at the support periphery minimizes steric confinement effects, allowing simultaneous product desorption and oxygen adsorption – a critical advantage for sustaining continuous catalytic cycles. Through combined experimental and theoretical analyses, it is demonstrated that this dual-channel electron transport system effectively reduces activation barriers for elementary steps while accelerating charge transfer kinetics. This fundamental study establishes a new paradigm for designing high-performance ORR catalysts through multi-site collaborative engineering and reaction pathway optimization.
期刊介绍:
Small serves as an exceptional platform for both experimental and theoretical studies in fundamental and applied interdisciplinary research at the nano- and microscale. The journal offers a compelling mix of peer-reviewed Research Articles, Reviews, Perspectives, and Comments.
With a remarkable 2022 Journal Impact Factor of 13.3 (Journal Citation Reports from Clarivate Analytics, 2023), Small remains among the top multidisciplinary journals, covering a wide range of topics at the interface of materials science, chemistry, physics, engineering, medicine, and biology.
Small's readership includes biochemists, biologists, biomedical scientists, chemists, engineers, information technologists, materials scientists, physicists, and theoreticians alike.