Heteroatom Dopants Promote Two-Electron O2 Reduction for Photocatalytic Production of H2O2 on Polymeric Carbon Nitride

Peng Zhang, Yawen Tong, Yong Liu, Junie Jhon M. Vequizo, Hongwei Sun, Can Yang, Akira Yamakata, Fengtao Fan, Wei Lin, Xinchen Wang, Wonyong Choi

Research output: Contribution to journalArticlepeer-review

109 Citations (Scopus)

Abstract

Polymeric carbon nitride modified with selected heteroatom dopants was prepared and used as a model photocatalyst to identify and understand the key mechanisms required for efficient photoproduction of H2O2 via selective oxygen reduction reaction (ORR). The photochemical production of H2O2 was achieved at a millimolar level per hour under visible-light irradiation along with 100 % apparent quantum yield (in 360–450 nm region) and 96 % selectivity in an electrochemical system (0.1 V vs. RHE). Spectroscopic analysis in spatiotemporal resolution and theoretical calculations revealed that the synergistic association of alkali and sulfur dopants in the polymeric matrix promoted the interlayer charge separation and polarization of trapped electrons for preferable oxygen capture and reduction in ORR kinetics. This work highlights the key features that are responsible for controlling the photocatalytic activity and selectivity toward the two-electron ORR, which should be the basis of further development of solar H2O2 production.

Original languageEnglish
Pages (from-to)16209-16217
Number of pages9
JournalAngewandte Chemie - International Edition
Volume59
Issue number37
DOIs
Publication statusPublished - Sep 7 2020
Externally publishedYes

Keywords

  • doping
  • HO production
  • oxygen reduction reaction
  • photocatalysts
  • solar fuel

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)

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