4.8 Article

Pyranoid-O-dominated graphene-like nanocarbon for two-electron oxygen reduction reaction

Journal

APPLIED CATALYSIS B-ENVIRONMENTAL
Volume 307, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apcatb.2022.121173

Keywords

Oxygen reduction reaction; Electrocatalyst; Carbonaceous materials; Two-electron selectivity; Hydrogen peroxide electrosynthesis

Funding

  1. National Natural Science Foundation of China [91963109]
  2. Foundation of State Key Laboratory of Coal Combustion [FSKLCCA2008]
  3. Open Found of Hubei Key Laboratory of Material Chemistry and Service Failure [2021MCF03]
  4. State Key Laboratory of Advanced Technology [2021-KF-4]
  5. Key Labo-ratory of Hubei Province for Coal Conversion and New Carbon Materials (Wuhan University of Science and Technology) [WKDM202101]

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In this study, a pyranoid-O-dominated graphene-like nanocarbon (GLC) material with high surface area, hierarchical porous structure, and abundant edge defects was successfully constructed through the high-temperature alkali activation of cellulose-based precursor. The GLC electrocatalyst exhibited excellent 2e- ORR performance with high H2O2 productivity and ultrafast wastewater degradation ability. These findings provide new insight into the 2e- ORR selectivity of carbon-based electrocatalysts for H2O2 production.
Exploring the high-efficient two-electron oxygen reduction reaction (2e- ORR) catalysts is greatly significant for promoting hydrogen peroxide (H2O2) electroproduction. Herein, we have constructed a pyranoid-O-dominated graphene-like nanocarbon (GLC) material with high surface area, hierarchical porous structure, and abundant edge defects, through the high-temperature alkali activation of cellulose-based precursor. Benefiting from its integrated merits, the GLC electrocatalyst exhibits excellent 2e- ORR performance with high H2O2 productivity and ultrafast wastewater degradation ability. Interestingly, whether changing the carbonaceous precursor or alkali activator, all the as-prepared pyranoid-O-dominated GLC-based materials display high 2e- selectivity for the ORR. Based on further analogical experiments and theoretical analysis, the results reveal that the nature of 2e- selectivity on carbon-based materials is highly associated with the pyranoid-O dopants, rather than the surface oxygen-containing functional groups declared by the previous reports. These findings may bring new insight into the 2e- ORR selectivity of carbon-based electrocatalysts for H2O2 production.

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