Electronic configuration inversion in CdIn2S4 for efficient photocatalytic hydrogen peroxide generation coupled with selective benzylamine oxidation.
J Colloid Interface Sci
; 656: 528-537, 2024 Feb 15.
Article
em En
| MEDLINE
| ID: mdl-38007944
ABSTRACT
Vacancies engineering has sparked a huge interest in enhancing photocatalytic activity, but monovacancy simultaneously conducts as either electron or hole acceptor and redox reaction, worsening charge transfer and catalytic performance. Here, the concept of electronic inversion has been proposed through the simultaneous introduction of surface oxygen and S vacancies in CdIn2S4 (OSv-CIS). Consequently, under mild conditions, the well-designed OSv-CIS-200 demonstrated a strong rate of N-benzylidenebenzylamine production (2972.07 µmol g-1 h-1) coupled with Hydrogen peroxide (H2O2) synthesis (2362.33 µmol g-1 h-1) (PIH), which is 12.4 times higher than that of CdIn2S4. Density functional theory (DFT) simulation and characterization studies demonstrate that oxygen is introduced into the lattice on the surface of the material, reversing the charge distribution of the S vacancy and enhancing the polarity of the total charge distribution. It not only provides a huge built-in electric field (BEF) for guiding the orientation of the charge transfer, but also acts as a long-distance active site to accelerate reaction and prevent H2O2 decomposition. Our work offers a straightforward connection between the atomic defect and intrinsic properties for designing high-efficiency materials.
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Coleções:
01-internacional
Base de dados:
MEDLINE
Idioma:
En
Revista:
J Colloid Interface Sci
Ano de publicação:
2024
Tipo de documento:
Article