Spatially separating redox centers on 2D carbon nitride with cobalt single atom for photocatalytic H2O2 production

Chiheng Chu, Qianhong Zhu, Zhenhua Pan, Srishti Gupta, Dahong Huang, Yonghua Du, Seunghyun Weon, Yueshen Wu, Christopher Muhich, Eli Stavitski, Kazunari Domen, Jae Hong Kim

Research output: Contribution to journalArticle

3 Scopus citations

Abstract

Redox cocatalysts play crucial roles in photosynthetic reactions, yet simultaneous loading of oxidative and reductive cocatalysts often leads to enhanced charge recombination that is detrimental to photosynthesis. This study introduces an approach to simultaneously load two redox cocatalysts, atomically dispersed cobalt for improving oxidation activity and anthraquinone for improving reduction selectivity, onto graphitic carbon nitride (C3N4) nanosheets for photocatalytic H2O2 production. Spatial separation of oxidative and reductive cocatalysts was achieved on a two-dimensional (2D) photocatalyst, by coordinating cobalt single atom above the void center of C3N4 and anchoring anthraquinone at the edges of C3N4 nanosheets. Such spatial separation, experimentally confirmed and computationally simulated, was found to be critical for enhancing surface charge separation and achieving efficient H2O2 production. This center/edge strategy for spatial separation of cocatalysts may be applied on other 2D photocatalysts that are increasingly studied in photosynthetic reactions.

Original languageEnglish (US)
Pages (from-to)6376-6382
Number of pages7
JournalProceedings of the National Academy of Sciences of the United States of America
Volume117
Issue number12
DOIs
StatePublished - Mar 24 2020

Keywords

  • 2D photocatalyst
  • Hydrogen peroxide
  • Single-atom catalyst
  • Spatially separated cocatalysts

ASJC Scopus subject areas

  • General

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