COF/In2S3 S‐Scheme Photocatalyst with Enhanced Light Absorption and H2O2‐Production Activity and fs‐TA Investigation
Authors:
Top Cited Papers
- 10 March 2024
- journal article
- research article
- Published by Wiley in Advanced Materials
- Vol. 36 (24) , e2400288
Abstract
Photocatalytic hydrogen peroxide (H2O2) synthesis from water and O2 is an economical, eco‐friendly, and sustainable route for H2O2 production. However, single‐component photocatalysts are subjected to limited light‐harvesting range, fast carrier recombination, and weak redox power. To promote photogenerated carrier separation and enhance redox abilities, an organic/inorganic S‐scheme photocatalyst is fabricated by in situ growing In2S3 nanosheets on a covalent organic framwork (COF) substrate for efficient H2O2 production in pure water. Interestingly, compared to unitary COF and In2S3, the COF/In2S3 S‐scheme photocatalysts exhibit significantly larger light‐harvesting range and stronger visible‐light absorption. Partial density of state calculation, X‐ray photoelectron spectroscopy, and femtosecond transient absorption spectroscopy reveal that the coordination between In2S3 and COF induces the formation of mid‐gap hybrid energy levels, leading to smaller energy gaps and broadened absorption. Combining electron spin resonance spectroscopy, radical‐trapping experiments, and isotope labeling experiments, three pathways for H2O2 formation are identified. Benefited from expanded light‐absorption range, enhanced carrier separation, strong redox power, and multichannel H2O2 formation, the optimal composite shows an impressive H2O2‐production rate of 5713.2 µmol g−1 h−1 in pure water. This work exemplifies an effective strategy to ameliorate COF‐based photocatalysts by building S‐scheme heterojunctions and provides molecular‐level insights into their impact on energy level modulation.Keywords
Funding Information
- National Key Research and Development Program of China (2022YFB3803600, 2022YFE0115900)
- National Natural Science Foundation of China (22208332, 52073223, 22278324, 51932007, 22238009, 22261142666, 22361142704)
This publication has 60 references indexed in Scilit:
- Sulfone‐Modified Covalent Organic Frameworks Enabling Efficient Photocatalytic Hydrogen Peroxide Generation via One‐Step Two‐Electron O2 ReductionAngewandte Chemie International Edition, 2023
- Verifying the Charge‐Transfer Mechanism in S‐Scheme Heterojunctions Using Femtosecond Transient Absorption SpectroscopyAngewandte Chemie International Edition, 2023
- Modulating the Band Structure of Metal Coordinated Salen COFs and an In Situ Constructed Charge Transfer Heterostructure for Electrocatalysis Hydrogen EvolutionAdvanced Science, 2022
- Inorganic Metal‐Oxide Photocatalyst for H2O2 ProductionSmall, 2021
- Enhanced Mass Transfer of Oxygen through a Gas–Liquid–Solid Interface for Photocatalytic Hydrogen Peroxide ProductionAdvanced Functional Materials, 2021
- Construction of Core–Shell MOF@COF Hybrids with Controllable Morphology Adjustment of COF Shell as a Novel Platform for Photocatalytic Cascade ReactionsAdvanced Science, 2021
- Pyrimidine‐Functionalized Covalent Organic Framework and its Cobalt Complex as an Efficient Electrocatalyst for Oxygen Evolution ReactionChemSusChem, 2021
- An Inorganic/Organic S‐Scheme Heterojunction H2‐Production Photocatalyst and its Charge Transfer MechanismAdvanced Materials, 2021
- Electrochemical and Photoelectrochemical Water Oxidation for Hydrogen Peroxide ProductionAngewandte Chemie International Edition, 2020
- Acetylene and Diacetylene Functionalized Covalent Triazine Frameworks as Metal‐Free Photocatalysts for Hydrogen Peroxide Production: A New Two‐Electron Water Oxidation PathwayAdvanced Materials, 2019