In-Plane Topological-Defect-Enriched Graphene as an Efficient Metal-Free Catalyst for pH-Universal H2O2 Electrosynthesis.
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; 20(29): e2400564, 2024 Jul.
Article
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| MEDLINE
| ID: mdl-38368264
ABSTRACT
Developing efficient metal-free catalysts to directly synthesize hydrogen peroxide (H2O2) 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 SâCâN motifs, which effectively modulates atomic and electronic structures of graphene. The SNC catalyst delivers ultrahigh H2O2 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 SâCâN motifs efficiently optimize the binding strength to OOH* intermediate and substantially diminish the kinetic barrier for reducing O2 to H2O2, thereby promoting the intrinsic activity of 2e-ORR.
Texto completo:
1
Colección:
01-internacional
Banco de datos:
MEDLINE
Idioma:
En
Revista:
Small
Asunto de la revista:
ENGENHARIA BIOMEDICA
Año:
2024
Tipo del documento:
Article
País de afiliación:
China