Boosting photocatalytic hydrogen peroxide production by regulating electronic configuration of single Sb atoms via carbon vacancies in carbon nitrides

Qinye He, Jie Ding, Hsin Jung Tsai, Yuhang Liu, Min Wei, Qiao Zhang, Zhiming Wei, Zhaoyang Chen, Jian Huang, Sung Fu Hung*, Hongbin Yang, Yueming Zhai

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

2 Scopus citations

Abstract

Single-atom catalysts supported on semiconductors can serve as active sites for efficient oxygen reduction to hydrogen peroxide (H2O2). However, researchers have long been puzzled by the lack of guidance on optimizing the performance of single-atom photocatalysts. In this study, we propose a versatile strategy that utilizes carbon vacancies to regulate the electronic configuration of antimony (Sb) atoms on carbon nitrides (C3N4). This strategy has been found to significantly enhance the photocatalytic production of H2O2. The H2O2 evolution rate of Sb single-atom on carbon vacancy-rich C3N4 (designated as Sb1/Cv-C3N4) is 5.369 mmol g-1h−1, which is 10.9 times higher than C3N4 alone. By combining experimental characterizations and density functional theory simulations, we reveal the strong electronic interaction between Sb atoms and carbon vacancy-rich C3N4. This interaction is capable for maintaining the electron-rich state of Sb atoms, facilitating efficient electron transfer to pauling-type absorbed oxygen, and ultimately enhancing the formation of *OOH intermediates. This innovative defect-engineering approach can manipulate the electronic configuration of single-atom catalysts, providing a new avenue to boost the photocatalytic oxygen reduction reaction towards H2O2 production.

Original languageEnglish
Pages (from-to)18-26
Number of pages9
JournalJournal of Colloid And Interface Science
Volume651
DOIs
StatePublished - Dec 2023

Keywords

  • Carbon nitride
  • Carbon vacancy
  • Electronic configuration
  • Hydrogen peroxide
  • Single-atom catalyst

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