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Vol. 15 (2023)

Metal-Free 2D/2D van der Waals Heterojunction Based on Covalent Organic Frameworks for Highly Efficient Solar Energy Catalysis

https://doi.org/10.1007/s40820-023-01100-x
Ge Yan
Institute of Clean Energy Chemistry, Key Laboratory for Green Synthesis and Preparative Chemistry of Adv. Mater., College of Chemistry, Liaoning University, Shenyang 110036, People’s Republic of China
Xiaodong Sun
Institute of Clean Energy Chemistry, Key Laboratory for Green Synthesis and Preparative Chemistry of Adv. Mater., College of Chemistry, Liaoning University, Shenyang 110036, People’s Republic of China
Yu Zhang
Institute of Clean Energy Chemistry, Key Laboratory for Green Synthesis and Preparative Chemistry of Adv. Mater., College of Chemistry, Liaoning University, Shenyang 110036, People’s Republic of China
Hui Li
School of Science, RMIT University, Melbourne, VIC 3000, Australia
Hongwei Huang
Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid Wastes, National Laboratory of Mineral Materials, School of Materials Science and Technology, China University of Geosciences, Beijing 100083, People’s Republic of China
Baohua Jia
School of Science, RMIT University, Melbourne, VIC 3000, Australia
Dawei Su
Faculty of Science, School of Mathematical and Physical Sciences, University of Technology Sydney, Sydney, NSW 2007, Australia
Tianyi Ma
School of Science, RMIT University, Melbourne, VIC 3000, Australia

Corresponding Author: Tianyi Ma

tianyi.ma@rmit.edu.au

Nano-Micro Letters, Vol. 15 (2023), Article Number: 132

Abstract

Covalent organic frameworks (COFs) have emerged as a kind of rising star materials in photocatalysis. However, their photocatalytic activities are restricted by the high photogenerated electron–hole pairs recombination rate. Herein, a novel metal-free 2D/2D van der Waals heterojunction, composed of a two-dimensional (2D) COF with ketoenamine linkage (TpPa-1-COF) and 2D defective hexagonal boron nitride (h-BN), is successfully constructed through in situ solvothermal method. Benefitting from the presence of VDW heterojunction, larger contact area and intimate electronic coupling can be formed between the interface of TpPa-1-COF and defective h-BN, which make contributions to promoting charge carriers separation. The introduced defects can also endow the h-BN with porous structure, thus providing more reactive sites. Moreover, the TpPa-1-COF will undergo a structural transformation after being integrated with defective h-BN, which can enlarge the gap between the conduction band position of the h-BN and TpPa-1-COF, and suppress electron backflow, corroborated by experimental and density functional theory calculations results. Accordingly, the resulting porous h-BN/TpPa-1-COF metal-free VDW heterojunction displays outstanding solar energy catalytic activity for water splitting without co-catalysts, and the H2 evolution rate can reach up to 3.15 mmol g−1 h−1, which is about 67 times greater than that of pristine TpPa-1-COF, also surpassing that of state-of-the-art metal-free-based photocatalysts reported to date. In particular, it is the first work for constructing COFs-based heterojunctions with the help of h-BN, which may provide new avenue for designing highly efficient metal-free-based photocatalysts for H2 evolution.


Highlights:


1 It is the first attempt to combine covalent organic frameworks with hexagonal boron nitride (h-BN) to construct efficient metal-free photocatalyst.
2 The composite displays superior photocatalytic hydrogen production performance in metal-free systems.
3 The integrated porous h-BN can suppress electron backflow to optimize the composite photocatalytic activity.

Keywords

Covalent organic frameworks 2D/2D van der Waals heterojunction Metal-free photocatalyst
Yan, Ge, Xiaodong Sun, Yu Zhang, Hui Li, Hongwei Huang, Baohua Jia, Dawei Su, and Tianyi Ma. 2023. “Metal-Free 2D/2D Van Der Waals Heterojunction Based on Covalent Organic Frameworks for Highly Efficient Solar Energy Catalysis”. Nano-Micro Letters 15 (May):132. https://doi.org/10.1007/s40820-023-01100-x.
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