Jun-Fei Gu , Jichao Wang , Caixia Wang , Jin Li , Cheng Chen , Ni Zhang , Xiang-Ya Xu , Somboon Chaemchuen
{"title":"二维ZIF-L衍生的双Fe/FeNx位点在碱性和酸性介质中协同高效氧还原。","authors":"Jun-Fei Gu , Jichao Wang , Caixia Wang , Jin Li , Cheng Chen , Ni Zhang , Xiang-Ya Xu , Somboon Chaemchuen","doi":"10.1016/j.jcis.2025.01.089","DOIUrl":null,"url":null,"abstract":"<div><div>Fe–N–C catalysts have emerged as the most promising alternatives to commercial Pt/C catalysts for oxygen reduction reaction (ORR) due to their cost-effectiveness and favorable activity. Herein, a dual-site Fe/FeN<sub>x</sub>-NC catalyst was synthesized via a green, in situ doping strategy using two-dimensional Fe-doped ZIF-L as a nitrogen-rich precursor. The catalyst integrated Fe nanoparticles (NPs) and FeN<sub>x</sub> sites anchored on carbon nanotubes, intertwined with nitrogen-doped porous carbon nanosheets, achieving a high active site density and graphitisation. Electrochemical tests revealed that the optimized Fe/FeN<sub>x</sub>-NC-1 exhibited significant ORR activity, with a half-wave potential of 0.92 V and 0.80 V for alkaline and acidic medium, respectively. Zn-air batteries employing Fe/FeN<sub>x</sub>-NC-1 delivered a peak power density of 168 mW·cm<sup>−2</sup> and a specific capacity of 790 mAh·g<sup>−1</sup>, outperforming those of Pt-based catalysts. Density functional theory calculations demonstrated a reduced free energy barrier for the rate-determining step (0.48 eV) compared to single-site Fe–N<sub>4</sub> models (0.79 eV). The synergy between Fe NPs and FeN<sub>x</sub> optimized ORR intermediate adsorption and facilitated charge/mass transfer. This study offers valuable insights for the development of advanced energy conversion systems.</div></div>","PeriodicalId":351,"journal":{"name":"Journal of Colloid and Interface Science","volume":"684 ","pages":"Pages 159-169"},"PeriodicalIF":9.4000,"publicationDate":"2025-01-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Two-dimensional ZIF-L derived dual Fe/FeNx sites for synergistic efficient oxygen reduction in alkaline and acid media\",\"authors\":\"Jun-Fei Gu , Jichao Wang , Caixia Wang , Jin Li , Cheng Chen , Ni Zhang , Xiang-Ya Xu , Somboon Chaemchuen\",\"doi\":\"10.1016/j.jcis.2025.01.089\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Fe–N–C catalysts have emerged as the most promising alternatives to commercial Pt/C catalysts for oxygen reduction reaction (ORR) due to their cost-effectiveness and favorable activity. Herein, a dual-site Fe/FeN<sub>x</sub>-NC catalyst was synthesized via a green, in situ doping strategy using two-dimensional Fe-doped ZIF-L as a nitrogen-rich precursor. The catalyst integrated Fe nanoparticles (NPs) and FeN<sub>x</sub> sites anchored on carbon nanotubes, intertwined with nitrogen-doped porous carbon nanosheets, achieving a high active site density and graphitisation. Electrochemical tests revealed that the optimized Fe/FeN<sub>x</sub>-NC-1 exhibited significant ORR activity, with a half-wave potential of 0.92 V and 0.80 V for alkaline and acidic medium, respectively. Zn-air batteries employing Fe/FeN<sub>x</sub>-NC-1 delivered a peak power density of 168 mW·cm<sup>−2</sup> and a specific capacity of 790 mAh·g<sup>−1</sup>, outperforming those of Pt-based catalysts. Density functional theory calculations demonstrated a reduced free energy barrier for the rate-determining step (0.48 eV) compared to single-site Fe–N<sub>4</sub> models (0.79 eV). The synergy between Fe NPs and FeN<sub>x</sub> optimized ORR intermediate adsorption and facilitated charge/mass transfer. This study offers valuable insights for the development of advanced energy conversion systems.</div></div>\",\"PeriodicalId\":351,\"journal\":{\"name\":\"Journal of Colloid and Interface Science\",\"volume\":\"684 \",\"pages\":\"Pages 159-169\"},\"PeriodicalIF\":9.4000,\"publicationDate\":\"2025-01-13\",\"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://www.sciencedirect.com/science/article/pii/S0021979725001031\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Colloid and Interface Science","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0021979725001031","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Two-dimensional ZIF-L derived dual Fe/FeNx sites for synergistic efficient oxygen reduction in alkaline and acid media
Fe–N–C catalysts have emerged as the most promising alternatives to commercial Pt/C catalysts for oxygen reduction reaction (ORR) due to their cost-effectiveness and favorable activity. Herein, a dual-site Fe/FeNx-NC catalyst was synthesized via a green, in situ doping strategy using two-dimensional Fe-doped ZIF-L as a nitrogen-rich precursor. The catalyst integrated Fe nanoparticles (NPs) and FeNx sites anchored on carbon nanotubes, intertwined with nitrogen-doped porous carbon nanosheets, achieving a high active site density and graphitisation. Electrochemical tests revealed that the optimized Fe/FeNx-NC-1 exhibited significant ORR activity, with a half-wave potential of 0.92 V and 0.80 V for alkaline and acidic medium, respectively. Zn-air batteries employing Fe/FeNx-NC-1 delivered a peak power density of 168 mW·cm−2 and a specific capacity of 790 mAh·g−1, outperforming those of Pt-based catalysts. Density functional theory calculations demonstrated a reduced free energy barrier for the rate-determining step (0.48 eV) compared to single-site Fe–N4 models (0.79 eV). The synergy between Fe NPs and FeNx optimized ORR intermediate adsorption and facilitated charge/mass transfer. This study offers valuable insights for the development of advanced energy conversion systems.
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