Dual Regulation of Charge Separation and the Oxygen Reduction Pathway by Encapsulating Phosphotungstic Acid into the Cationic Covalent Organic Framework for Efficient Photocatalytic Hydrogen Peroxide Production.
ACS Appl Mater Interfaces
; 16(5): 5758-5768, 2024 Feb 07.
Article
en En
| MEDLINE
| ID: mdl-38273463
ABSTRACT
Previous research on covalent organic framework (COF)-based photocatalytic H2O2 synthesis from oxygen reduction focuses more on charge carrier separation but less on the electron utilization efficiency of O2. Herein, we put forward a facile approach to simultaneously promote charge separation and tailor the oxygen reduction pathway by introducing phosphotungstic acid (PTA) into the cationic COF skeleton. Experiments verified that PTA, as an electron transport medium, establishes a fast electron transfer channel from the COF semiconductor conductor band to the substrate O2; meanwhile, the reaction path is optimized by its catalytic cycle for preferable dioxygen capture and reduction in oxygen reduction reaction (ORR) kinetics. The existence of PTA promotes the rate and tendency of converting O2 into â¢O2- intermediates, which is conducive to boosting the photocatalytic activity and selectivity toward the sequential two-step single-electron ORR. As expected, compared to the pristine TTB-EB, the optimal PTA0.5@TTB-EB achieves a 2.2-fold improvement of visible-light-driven photocatalytic performance with a H2O2 production rate of 897.94 µmol·L-1·h-1 in pure water without using any sacrificial agents. In addition, owing to the robust electrostatic interaction and the confinement effect of porous TTB-EB channels, the PTA@TTB-EB composite possessed favorable stability.
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1
Colección:
01-internacional
Base de datos:
MEDLINE
Idioma:
En
Revista:
ACS Appl Mater Interfaces
Asunto de la revista:
BIOTECNOLOGIA
/
ENGENHARIA BIOMEDICA
Año:
2024
Tipo del documento:
Article
País de afiliación:
China
Pais de publicación:
Estados Unidos