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[NTU-BDA-THTA] COFs with Covalently Bridged Inorganic/Organic Hybrids toward Efficient Photocatalysis
Summary:
Professor Yanli Zhao's team from Nanyang Technological University in Singapore has developed a series of covalent organic frameworks (COFs) in this paper, in which the ratio of β-ketoenamine to imine bonds varies, making significant progress in photocatalytic hydrogen production.
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Background:
1. To address the challenge of low photocatalytic efficiency in pure COF photocatalysts due to fast charge recombination, previous researchers explored hybridization strategies, achieving some success. However, there were still problems such as insufficient charge separation and transfer efficiency. 2. The authors in this work proposed an innovative method of integrating suitable linkage evolution and covalent inorganic/organic heterostructure, obtaining remarkable results in improving photocatalytic performance.
Research Content:
1. Synthesis:
The authors synthesized three kinds of COFs (NTU-BDA-HTA, NTU-BDA-DHTA, and NTU-BDA-THTA) using an acid-catalyzed Schiff base reaction of benzene-1,4-diamine (BDA) with benzene-1,3,5-tricarbaldehyde derivatives bearing different numbers of hydroxy groups.
2. Characterizations:
1) The BET surface areas of NTU-BDA-HTA, NTU-BDA-DHTA, and NTU-BDA-THTA are 1289.3, 1344.2, and 768.0 m² g⁻¹, respectively, with a pore size of around 1.4 nm. 2) SEM/TEM tests show the particle size of the materials to be above 1 μm, with urchin-like, microsphere-like, and clavate-like morphologies, respectively. 3) Other electrochemical or optical tests reveal that the optical bandgaps are 1.81, 1.77, and 2.09 eV for NTU-BDA-HTA, NTU-BDA-DHTA, and NTU-BDA-THTA, respectively.
3. Application:
The materials were tested in photocatalytic hydrogen evolution under visible light (≥420 nm) with Pt and L-ascorbic acid as cocatalyst and sacrificial electron donor, respectively. The highest H₂ accumulation amount was obtained from NTU-BDA-THTA, followed by NTU-BDA-DHTA and NTU-BDA-HTA.
4. Mechanism:
The analysis of the experimental results indicates that the increase of HOMO energy with the increase of the β-ketoenamine linkage correlates with the observed photocatalytic trend. The excited state of mixed-linkage COFs may be suppressed by the imine moiety, impeding the photoredox process. The covalent integration of NTU-BDA-THTA with NH₂-Ti₃C₂Tx forms a heterojunction that facilitates efficient charge separation and transfer, contributing to enhanced photocatalytic activity.
Outlook:
This research demonstrates an effective strategy to construct COF-based photocatalysts by integrating linkage evolution and covalent inorganic/organic heterostructure. The findings provide valuable insights into the rational design of COFs for efficient photocatalytic applications and open up new avenues for the development of high-performance photocatalytic materials.
Integrating Suitable Linkage of Covalent-Organic Frameworks into Covalently Bridged Inorganic/Organic Hybrids toward Efficient Photocatalysis
Authors: Hou Wang, Cheng Qian, Jia Liu, Yongfei Zeng, Dongdong Wang, Weiqiang Zhou, Long Gu, Hongwei Wu, Guofeng Liu, Yanli Zhao
DOI: 10.1021/jacs.0c00054
Link: https://pubs.acs.org/doi/10.1021/jacs.0c00054
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