Iron clusters regulate local charge distribution in Fe-N4 sites to boost oxygen electroreduction
Copyright © 2023 Elsevier Inc. All rights reserved..
The atomically-dispersed and nitrogen-coordinated iron (FeNC) on a carbon catalyst is a potential non-noble metal catalyst that can replace precious metal electrocatalysts. However, its activity is often unsatisfactory owing to the symmetric charge distribution around the iron matrix. In this study, atomically- dispersed Fe-N4 and Fe nanoclusters loaded with N-doped porous carbon (FeNCs/FeSAs-NC-Z834) were rationally fabricated by introducing homologous metal clusters and increasing the N content of the support. FeNCs/FeSAs-NC-Z8@34 exhibited a half-wave potential of 0.918 V, which exceeded that of the commercial benchmark Pt/C catalyst. Theoretical calculations verified that introducing Fe nanoclusters can break the symmetric electronic structure of Fe-N4, thus inducing charge redistribution. Furthermore, it can optimize a part of Fe 3d occupancy orbitals and accelerate OO fracture in OOH* (rate-determining step), thus significantly improving oxygen reduction reaction activity. This work provides a reasonably advanced pathway to modulate the electronic structure of the single-atom center and optimize the catalytic activity of single-atom catalysts.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2023 |
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| Erschienen: |
2023 |
| Enthalten in: |
Zur Gesamtaufnahme - volume:648 |
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| Enthalten in: |
Journal of colloid and interface science - 648(2023) vom: 15. Okt., Seite 440-447 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Bai, Jirong [VerfasserIn] |
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| Links: |
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| Themen: |
Charge redistribution |
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| Anmerkungen: |
Date Completed 04.07.2023 Date Revised 04.07.2023 published: Print-Electronic Citation Status PubMed-not-MEDLINE |
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| doi: |
10.1016/j.jcis.2023.06.016 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM358039630 |
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| 500 | |a Date Revised 04.07.2023 | ||
| 500 | |a published: Print-Electronic | ||
| 500 | |a Citation Status PubMed-not-MEDLINE | ||
| 520 | |a Copyright © 2023 Elsevier Inc. All rights reserved. | ||
| 520 | |a The atomically-dispersed and nitrogen-coordinated iron (FeNC) on a carbon catalyst is a potential non-noble metal catalyst that can replace precious metal electrocatalysts. However, its activity is often unsatisfactory owing to the symmetric charge distribution around the iron matrix. In this study, atomically- dispersed Fe-N4 and Fe nanoclusters loaded with N-doped porous carbon (FeNCs/FeSAs-NC-Z834) were rationally fabricated by introducing homologous metal clusters and increasing the N content of the support. FeNCs/FeSAs-NC-Z8@34 exhibited a half-wave potential of 0.918 V, which exceeded that of the commercial benchmark Pt/C catalyst. Theoretical calculations verified that introducing Fe nanoclusters can break the symmetric electronic structure of Fe-N4, thus inducing charge redistribution. Furthermore, it can optimize a part of Fe 3d occupancy orbitals and accelerate OO fracture in OOH* (rate-determining step), thus significantly improving oxygen reduction reaction activity. This work provides a reasonably advanced pathway to modulate the electronic structure of the single-atom center and optimize the catalytic activity of single-atom catalysts | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a Charge redistribution | |
| 650 | 4 | |a Fe nanocluster | |
| 650 | 4 | |a Fe single atom | |
| 650 | 4 | |a Oxygen reduction reaction | |
| 650 | 4 | |a high content N | |
| 700 | 1 | |a Tang, Yiming |e verfasserin |4 aut | |
| 700 | 1 | |a Lin, Cheng |e verfasserin |4 aut | |
| 700 | 1 | |a Jiang, Xiankai |e verfasserin |4 aut | |
| 700 | 1 | |a Zhang, Chunyong |e verfasserin |4 aut | |
| 700 | 1 | |a Qin, Hengfei |e verfasserin |4 aut | |
| 700 | 1 | |a Zhou, Quanfa |e verfasserin |4 aut | |
| 700 | 1 | |a Xiang, Mei |e verfasserin |4 aut | |
| 700 | 1 | |a Lian, Yuebin |e verfasserin |4 aut | |
| 700 | 1 | |a Deng, Yaoyao |e verfasserin |4 aut | |
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