In-Plane Topological-Defect-Enriched Graphene as an Efficient Metal-Free Catalyst for pH-Universal H2 O2 Electrosynthesis
© 2024 Wiley-VCH GmbH..
Developing efficient metal-free catalysts to directly synthesize hydrogen peroxide (H2 O2 ) through a 2-electron (2e) oxygen reduction reaction (ORR) is crucial for substituting the traditional energy-intensive anthraquinone process. Here, in-plane topological defects enriched graphene with pentagon-S and pyrrolic-N coordination (SNC) is synthesized via the process of hydrothermal and nitridation. In SNC, pentagon-S and pyrrolic-N originating from thiourea precursor are covalently grafted onto the basal plane of the graphene framework, building unsymmetrical dumbbell-like S─C─N motifs, which effectively modulates atomic and electronic structures of graphene. The SNC catalyst delivers ultrahigh H2 O2 productivity of 8.1, 7.3, and 3.9 mol gcatalyst -1 h-1 in alkaline, neutral, and acidic electrolytes, respectively, together with long-term operational stability in pH-universal electrolytes, outperforming most reported carbon catalysts. Theoretical calculations further unveil that defective S─C─N motifs efficiently optimize the binding strength to OOH* intermediate and substantially diminish the kinetic barrier for reducing O2 to H2 O2 , thereby promoting the intrinsic activity of 2e-ORR.
| Medienart: |
E-Artikel |
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| Erscheinungsjahr: |
2024 |
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| Erschienen: |
2024 |
| Enthalten in: |
Zur Gesamtaufnahme - year:2024 |
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| Enthalten in: |
Small (Weinheim an der Bergstrasse, Germany) - (2024) vom: 17. Feb., Seite e2400564 |
| Sprache: |
Englisch |
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| Beteiligte Personen: |
Mou, Zhixing [VerfasserIn] |
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| Links: |
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| Themen: |
Electrosynthesis |
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| Anmerkungen: |
Date Revised 17.02.2024 published: Print-Electronic Citation Status Publisher |
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| doi: |
10.1002/smll.202400564 |
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| funding: |
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| Förderinstitution / Projekttitel: |
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| PPN (Katalog-ID): |
NLM368583236 |
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| 520 | |a © 2024 Wiley-VCH GmbH. | ||
| 520 | |a Developing efficient metal-free catalysts to directly synthesize hydrogen peroxide (H2 O2 ) through a 2-electron (2e) oxygen reduction reaction (ORR) is crucial for substituting the traditional energy-intensive anthraquinone process. Here, in-plane topological defects enriched graphene with pentagon-S and pyrrolic-N coordination (SNC) is synthesized via the process of hydrothermal and nitridation. In SNC, pentagon-S and pyrrolic-N originating from thiourea precursor are covalently grafted onto the basal plane of the graphene framework, building unsymmetrical dumbbell-like S─C─N motifs, which effectively modulates atomic and electronic structures of graphene. The SNC catalyst delivers ultrahigh H2 O2 productivity of 8.1, 7.3, and 3.9 mol gcatalyst -1 h-1 in alkaline, neutral, and acidic electrolytes, respectively, together with long-term operational stability in pH-universal electrolytes, outperforming most reported carbon catalysts. Theoretical calculations further unveil that defective S─C─N motifs efficiently optimize the binding strength to OOH* intermediate and substantially diminish the kinetic barrier for reducing O2 to H2 O2 , thereby promoting the intrinsic activity of 2e-ORR | ||
| 650 | 4 | |a Journal Article | |
| 650 | 4 | |a electrosynthesis | |
| 650 | 4 | |a graphene | |
| 650 | 4 | |a hydrogen peroxide (H2O2) | |
| 650 | 4 | |a metal-free catalyst | |
| 650 | 4 | |a topological defect | |
| 700 | 1 | |a Mu, Yuewen |e verfasserin |4 aut | |
| 700 | 1 | |a Liu, Lijia |e verfasserin |4 aut | |
| 700 | 1 | |a Cao, Daili |e verfasserin |4 aut | |
| 700 | 1 | |a Chen, Shuai |e verfasserin |4 aut | |
| 700 | 1 | |a Yan, Wenjun |e verfasserin |4 aut | |
| 700 | 1 | |a Zhou, Haiqing |e verfasserin |4 aut | |
| 700 | 1 | |a Chan, Ting-Shan |e verfasserin |4 aut | |
| 700 | 1 | |a Chang, Lo-Yueh |e verfasserin |4 aut | |
| 700 | 1 | |a Fan, Xiujun |e verfasserin |4 aut | |
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