Enhanced Selectivity in the Electroproduction of H2O2 via F/S Dual-Doping in Metal-Free Nanofibers

Fei Xiang, Xuhong Zhao, Jian Yang*, Ning Li, Wenxiao Gong, Yizhen Liu, Arturo Burguete-Lopez, Yulan Li, Xiaobin Niu*, Andrea Fratalocchi*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

21 Scopus citations

Abstract

Electrocatalytic two-electron oxygen reduction (2e ORR) to hydrogen peroxide (H2O2) is attracting broad interest in diversified areas including paper manufacturing, wastewater treatment, production of liquid fuels, and public sanitation. Current efforts focus on researching low-cost, large-scale, and sustainable electrocatalysts with high activity and selectivity. Here a large-scale H2O2 electrocatalysts based on metal-free carbon fibers with a fluorine and sulfur dual-doping strategy is engineered. Optimized samples yield with a high onset potential of 0.814 V versus reversible hydrogen electrode (RHE), an almost ideal 2e pathway selectivity of 99.1%, outperforming most of the recently reported carbon-based or metal-based electrocatalysts. First principle theoretical computations and experiments demonstrate that the intermolecular charge transfer coupled with electron spin redistribution from fluorine and sulfur dual-doping is the crucial factor contributing to the enhanced performances in 2e ORR. This work opens the door to the design and implementation of scalable, earth-abundant, highly selective electrocatalysts for H2O2 production and other catalytic fields of industrial interest.

Original languageEnglish (US)
Article number2208533
JournalAdvanced Materials
Volume35
Issue number7
DOIs
StatePublished - Feb 16 2023

Bibliographical note

Publisher Copyright:
© 2022 Wiley-VCH GmbH.

Keywords

  • heteroatom doping
  • hydrogen peroxide
  • metal-free electrocatalysts
  • selectivity
  • synergistic effect

ASJC Scopus subject areas

  • General Materials Science
  • Mechanics of Materials
  • Mechanical Engineering

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