{"title":"多孔铁双金属原子位诱导界面氢键的高效氧还原反应。","authors":"Jingwen Wang, Qing Zhang, Lin Yang, Chuangang Hu, Zhengyu Bai, Zhongwei Chen","doi":"10.1016/j.jcis.2024.12.119","DOIUrl":null,"url":null,"abstract":"<p><p>Interfacial hydrogen bonds are pivotal in enhancing proton activity and accelerating the kinetics of proton-coupled electron transfer during electrocatalytic oxygen reduction reaction (ORR). Here we propose a novel FeCr bimetallic atomic sites catalyst supported on a honeycomb-like porous carbon layer, designed to optimize the microenvironment for efficient electrocatalytic ORR through the induction of interfacial hydrogen bonds. Characterizations, including X-ray absorption spectroscopy and in situ infrared spectroscopy, disclose the rearrangement of delocalized electrons due to the formation of FeCr sites, which facilitates the dissociation of interfacial water molecules and the subsequent formation of hydrogen bonds. This process significantly accelerates the proton-coupled electron transfer process and enhances the ORR reaction kinetics. As a result, the catalyst FeCrNC achieves a remarkable half-wave potential of 0.92 V and exhibits superior four-electron selectivity in 0.1 M KOH solution. Moreover, the zinc-air battery assembled by FeCrNC demonstrates a high power density of 207 mW cm<sup>-2</sup> and negligible degradation over 240 h at a current density of 10 mA cm<sup>-2</sup>.</p>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"683 Pt 1","pages":"742-751"},"PeriodicalIF":9.4000,"publicationDate":"2025-04-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Interfacial hydrogen bonds induced by porous FeCr bimetallic atomic sites for efficient oxygen reduction reaction.\",\"authors\":\"Jingwen Wang, Qing Zhang, Lin Yang, Chuangang Hu, Zhengyu Bai, Zhongwei Chen\",\"doi\":\"10.1016/j.jcis.2024.12.119\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Interfacial hydrogen bonds are pivotal in enhancing proton activity and accelerating the kinetics of proton-coupled electron transfer during electrocatalytic oxygen reduction reaction (ORR). Here we propose a novel FeCr bimetallic atomic sites catalyst supported on a honeycomb-like porous carbon layer, designed to optimize the microenvironment for efficient electrocatalytic ORR through the induction of interfacial hydrogen bonds. Characterizations, including X-ray absorption spectroscopy and in situ infrared spectroscopy, disclose the rearrangement of delocalized electrons due to the formation of FeCr sites, which facilitates the dissociation of interfacial water molecules and the subsequent formation of hydrogen bonds. This process significantly accelerates the proton-coupled electron transfer process and enhances the ORR reaction kinetics. As a result, the catalyst FeCrNC achieves a remarkable half-wave potential of 0.92 V and exhibits superior four-electron selectivity in 0.1 M KOH solution. Moreover, the zinc-air battery assembled by FeCrNC demonstrates a high power density of 207 mW cm<sup>-2</sup> and negligible degradation over 240 h at a current density of 10 mA cm<sup>-2</sup>.</p>\",\"PeriodicalId\":351,\"journal\":{\"name\":\"Journal of Colloid and Interface Science\",\"volume\":\"683 Pt 1\",\"pages\":\"742-751\"},\"PeriodicalIF\":9.4000,\"publicationDate\":\"2025-04-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Colloid and Interface Science\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1016/j.jcis.2024.12.119\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2024/12/17 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Colloid and Interface Science","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1016/j.jcis.2024.12.119","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2024/12/17 0:00:00","PubModel":"Epub","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
在电催化氧还原反应(ORR)中,界面氢键是提高质子活性和加速质子耦合电子转移动力学的关键。在这里,我们提出了一种新型的fer双金属原子位催化剂,支撑在蜂窝状多孔碳层上,旨在通过诱导界面氢键来优化微环境,以实现高效的电催化ORR。表征,包括x射线吸收光谱和原位红外光谱,揭示了由于FeCr位点的形成而导致的离域电子的重排,这有利于界面水分子的解离和随后氢键的形成。该过程显著加快了质子耦合电子转移过程,提高了ORR反应动力学。结果表明,在0.1 M KOH溶液中,FeCrNC的半波电位达到了0.92 V,并表现出优异的四电子选择性。此外,由FeCrNC组装的锌-空气电池具有207 mW cm-2的高功率密度,在电流密度为10 mA cm-2的情况下,240 h的降解可以忽略不计。
Interfacial hydrogen bonds induced by porous FeCr bimetallic atomic sites for efficient oxygen reduction reaction.
Interfacial hydrogen bonds are pivotal in enhancing proton activity and accelerating the kinetics of proton-coupled electron transfer during electrocatalytic oxygen reduction reaction (ORR). Here we propose a novel FeCr bimetallic atomic sites catalyst supported on a honeycomb-like porous carbon layer, designed to optimize the microenvironment for efficient electrocatalytic ORR through the induction of interfacial hydrogen bonds. Characterizations, including X-ray absorption spectroscopy and in situ infrared spectroscopy, disclose the rearrangement of delocalized electrons due to the formation of FeCr sites, which facilitates the dissociation of interfacial water molecules and the subsequent formation of hydrogen bonds. This process significantly accelerates the proton-coupled electron transfer process and enhances the ORR reaction kinetics. As a result, the catalyst FeCrNC achieves a remarkable half-wave potential of 0.92 V and exhibits superior four-electron selectivity in 0.1 M KOH solution. Moreover, the zinc-air battery assembled by FeCrNC demonstrates a high power density of 207 mW cm-2 and negligible degradation over 240 h at a current density of 10 mA cm-2.
期刊介绍:
The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality.
Emphasis:
The journal emphasizes fundamental scientific innovation within the following categories:
A.Colloidal Materials and Nanomaterials
B.Soft Colloidal and Self-Assembly Systems
C.Adsorption, Catalysis, and Electrochemistry
D.Interfacial Processes, Capillarity, and Wetting
E.Biomaterials and Nanomedicine
F.Energy Conversion and Storage, and Environmental Technologies