Constructing benzothiadiazole‐based donor‒acceptor covalent organic frameworks for efficient photocatalytic H2 evolution
Abstract Donor‒acceptor covalent organic frameworks (D‒A COFs) have been regarded as promising materials for photocatalytic water splitting because of their tunable band gaps. However, their efficiency is hindered by fast charge recombination and low photostability. Herein, we proposed a donor struc...
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2025-01-01
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| author | Yanchang Huang Bin Gao Qihang Huang De‐Li Ma Hongwei Wu Cheng Qian |
| author_facet | Yanchang Huang Bin Gao Qihang Huang De‐Li Ma Hongwei Wu Cheng Qian |
| author_sort | Yanchang Huang |
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| description | Abstract Donor‒acceptor covalent organic frameworks (D‒A COFs) have been regarded as promising materials for photocatalytic water splitting because of their tunable band gaps. However, their efficiency is hindered by fast charge recombination and low photostability. Herein, we proposed a donor structural engineering strategy for improving the photocatalytic activity of D‒A COFs to tackle these problems. Two benzothiadiazole‐based D‒A COFs (DHU‐COF‐BB and DHU‐COF‐BP) with distinct donors were prepared for photocatalytic H2 evolution reaction (HER). As a comparison, DHU‐COF‐TB without benzothiadiazole moieties was also designed and synthesized. Impressively, the photocatalytic H2 production rate of DHU‐COF‐BB reaches 12.80 mmol g−1 h−1 under visible light irradiation (≥420 nm), which was nearly 2.0 and 3.1 times higher than that of DHU‐COF‐BP (6.47 mmol g−1 h−1) and DHU‐COF‐TB (4.06 mmol g−1 h−1), respectively. In addition, the apparent quantum efficiency (AQE) of DHU‐COF‐BB was up to 5.04% at 420 nm. Photocatalytic and electrochemical measurements indicate that the enhanced hydrogen evolution activity of DHU‐COF‐BB can be ascribed to the introduction of appropriate benzene moiety into the donors, which increases the charge separation efficiency and thereby suppresses the electron‒hole recombination. Density functional theory (DFT) calculations revealed that both triphenylamine and benzothiadiazole units are the main active sites for HER over the DHU‐COF‐BB. This work provides new insight into the photocatalytic hydrogen production activity of D‒A COFs by a donor structural engineering strategy. |
| format | Article |
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| publishDate | 2025-01-01 |
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| spelling | doaj-art-dbe8321182bb45d3ad87701a7c58c8d52025-01-21T08:57:08ZengWileyAggregate2692-45602025-01-0161n/an/a10.1002/agt2.669Constructing benzothiadiazole‐based donor‒acceptor covalent organic frameworks for efficient photocatalytic H2 evolutionYanchang Huang0Bin Gao1Qihang Huang2De‐Li Ma3Hongwei Wu4Cheng Qian5State Key Laboratory for Modification of Chemical Fiber and Polymer Materials Key Laboratory of Science and Technology of Eco‐Textile, Ministry of Education, College of Chemistry and Chemical Engineering Donghua University Shanghai ChinaNational Laboratory of Solid State Microstructures College of Engineering and Applied Sciences Nanjing University Nanjing ChinaState Key Laboratory for Modification of Chemical Fiber and Polymer Materials Key Laboratory of Science and Technology of Eco‐Textile, Ministry of Education, College of Chemistry and Chemical Engineering Donghua University Shanghai ChinaState Key Laboratory for Modification of Chemical Fiber and Polymer Materials Key Laboratory of Science and Technology of Eco‐Textile, Ministry of Education, College of Chemistry and Chemical Engineering Donghua University Shanghai ChinaState Key Laboratory for Modification of Chemical Fiber and Polymer Materials Key Laboratory of Science and Technology of Eco‐Textile, Ministry of Education, College of Chemistry and Chemical Engineering Donghua University Shanghai ChinaState Key Laboratory for Modification of Chemical Fiber and Polymer Materials Key Laboratory of Science and Technology of Eco‐Textile, Ministry of Education, College of Chemistry and Chemical Engineering Donghua University Shanghai ChinaAbstract Donor‒acceptor covalent organic frameworks (D‒A COFs) have been regarded as promising materials for photocatalytic water splitting because of their tunable band gaps. However, their efficiency is hindered by fast charge recombination and low photostability. Herein, we proposed a donor structural engineering strategy for improving the photocatalytic activity of D‒A COFs to tackle these problems. Two benzothiadiazole‐based D‒A COFs (DHU‐COF‐BB and DHU‐COF‐BP) with distinct donors were prepared for photocatalytic H2 evolution reaction (HER). As a comparison, DHU‐COF‐TB without benzothiadiazole moieties was also designed and synthesized. Impressively, the photocatalytic H2 production rate of DHU‐COF‐BB reaches 12.80 mmol g−1 h−1 under visible light irradiation (≥420 nm), which was nearly 2.0 and 3.1 times higher than that of DHU‐COF‐BP (6.47 mmol g−1 h−1) and DHU‐COF‐TB (4.06 mmol g−1 h−1), respectively. In addition, the apparent quantum efficiency (AQE) of DHU‐COF‐BB was up to 5.04% at 420 nm. Photocatalytic and electrochemical measurements indicate that the enhanced hydrogen evolution activity of DHU‐COF‐BB can be ascribed to the introduction of appropriate benzene moiety into the donors, which increases the charge separation efficiency and thereby suppresses the electron‒hole recombination. Density functional theory (DFT) calculations revealed that both triphenylamine and benzothiadiazole units are the main active sites for HER over the DHU‐COF‐BB. This work provides new insight into the photocatalytic hydrogen production activity of D‒A COFs by a donor structural engineering strategy.https://doi.org/10.1002/agt2.669benzothiadiazolecovalent organic frameworkdonor‒acceptorphotocatalytic hydrogen evolution |
| spellingShingle | Yanchang Huang Bin Gao Qihang Huang De‐Li Ma Hongwei Wu Cheng Qian Constructing benzothiadiazole‐based donor‒acceptor covalent organic frameworks for efficient photocatalytic H2 evolution Aggregate benzothiadiazole covalent organic framework donor‒acceptor photocatalytic hydrogen evolution |
| title | Constructing benzothiadiazole‐based donor‒acceptor covalent organic frameworks for efficient photocatalytic H2 evolution |
| title_full | Constructing benzothiadiazole‐based donor‒acceptor covalent organic frameworks for efficient photocatalytic H2 evolution |
| title_fullStr | Constructing benzothiadiazole‐based donor‒acceptor covalent organic frameworks for efficient photocatalytic H2 evolution |
| title_full_unstemmed | Constructing benzothiadiazole‐based donor‒acceptor covalent organic frameworks for efficient photocatalytic H2 evolution |
| title_short | Constructing benzothiadiazole‐based donor‒acceptor covalent organic frameworks for efficient photocatalytic H2 evolution |
| title_sort | constructing benzothiadiazole based donor acceptor covalent organic frameworks for efficient photocatalytic h2 evolution |
| topic | benzothiadiazole covalent organic framework donor‒acceptor photocatalytic hydrogen evolution |
| url | https://doi.org/10.1002/agt2.669 |
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