4.8 Article

Synthesis of monolayer carbon-coated TiO2 as visible-light-responsive photocatalysts

Journal

APPLIED MATERIALS TODAY
Volume 27, Issue -, Pages -

Publisher

ELSEVIER
DOI: 10.1016/j.apmt.2022.101498

Keywords

Monolayer carbon shell; TiO2; Visible light absorption; Water-splitting; Dye degradation

Funding

  1. National Natural Science Foundation of China [51402314, 51972045, 51802316, 51927803]
  2. Sichuan Science and Technology Program [2021YFG0373]
  3. Funda-mental Research Funds for the Chinese Central Universities, China [ZYGX2019J025]
  4. Vice-Chancellor fellowship scheme at RMIT University
  5. ARC Centre of Excellence in Future Low-Energy Electronics Technologies (FLEET) [CE170100039]
  6. RMIT Micro Nano Research Facility (MNRF) in the Victorian node of the Australian National Fabrication Facility (ANFF)
  7. RMIT Microscopy and Microanalysis Facility (RMMF)

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A novel ultrasmall visible-light-responsive TiO2 photocatalyst with a hybrid structure and a monolayer carbon shell has been developed through chemical vapor deposition. The resulting structure possesses a narrowed bandgap and exhibits outstanding photocatalytic activity under visible light. The design also stabilizes Ti3+, facilitates the separation of photo-induced carriers, and enriches absorbing sites for target pollutants.
Increasing visible light absorption and constructing an active surface for TiO2 have long been pursued to obtain high photocatalytic activities. Modifying TiO2 at an atomic scale is desirable to optimize its surface state and band structure but remains a huge challenge. Herein, we developed an ultrasmall (similar to 5 nm) visible-light-responsive TiO2 photocatalyst with a novel hybrid structure (TiO2/C) through a chemical vapor deposition process on large scale. Environmental in-situ transmission electron microscope studies confirmed the anatase TiO2 with a monolayer carbon shell in a hybrid structure. The resulted structure possesses narrowed bandgap 2.83 eV, favoring the enhanced visible-light-responsive photocatalytic activity. Density functional theory (DFT) simulations confirm the tunable mechanism of carbon-induced localized energy band within the bandgap of TiO2. As a physical barrier without turning TiO2 black, the monolayer carbon shell stabilizes Ti3+ inside TiO2, facilitates the separation of photo-induced carriers and enriches abundant absorbing sites of target pollutants. Consequently, the TiO2/C exhibits outstanding photocatalytic performance in both photoelectrochemical water oxidation and dye degradation under visible light besides superior activity for hydrogen evolution under simulated sunlight irradiation. This design proved a meaningful strategy in obtaining visible-light-responsive photocatalysts with a stable active surface for industrial application.

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