Tang Qingmei, Wan Yuqi, Pan Zhiquan, Cheng Qingrong
Engineering Research Center of Phosphorous Development and Utilization of Ministry of Education, Wuhan Institute of Technology, Wuhan, 430205, PR China.
Engineering Research Center of Phosphorous Development and Utilization of Ministry of Education, Wuhan Institute of Technology, Wuhan, 430205, PR China; The Department of Electrical and Electronic Engineering, The University of Hong Kong, Hong Kong, 999077, PR China.
Environ Res. 2025 Mar 15;269:120901. doi: 10.1016/j.envres.2025.120901. Epub 2025 Jan 18.
S-scheme heterojunction is an effective tactic to improve photocatalytic property. But few studies on constructing heterojunction with BiOBr and covalent organic frameworks (COFs) are available. Herein, a novel series of COF-TpTt@BiOBr S-scheme heterojunctions with oxygen vacancies (OVs) were constructed via solvothermal method. COF-TpTt@BiOBr-10% showed enhanced photocatalytic performance under visible light. Pollutants (such as Methyl Orange (MO), methylene blue (MB), Rhodamine B (RhB), tetracycline (TC) and Levofloxacin hydrochloride (LEV)) can be efficiently degraded and the photocatalytic H generation rate reached 10828.075 μmol g h, which was 12.4 and 8.5 times of COF-TpTt and BiOBr. In addition, 3,3',5,5'-tetramethylbenzidine (TMB) oxidation experiment showed it has excellent molecular oxygen activation capacity. Furthermore, the S-scheme heterojunction charge transfer mechanism was proved by density functional theory (DFT) calculations. Under the influence of internal electric field, energy band bending and Coulomb force, e and h were efficiently separated and transferred. The formation of S-scheme heterojunction and generation of multiple free radicals assured the high redox activity of COF-TpTt@BiOBr-10% photocatalytic system. This study strengthened our deep understanding of S-scheme heterojunction charge transfer mechanism and offered a new way for high efficient hydrogen energy production.
S型异质结是提高光催化性能的有效策略。但关于构建BiOBr与共价有机框架（COF）异质结的研究较少。在此，通过溶剂热法构建了一系列具有氧空位（OVs）的新型COF-TpTt@BiOBr S型异质结。COF-TpTt@BiOBr-10%在可见光下表现出增强的光催化性能。污染物（如甲基橙（MO）、亚甲基蓝（MB）、罗丹明B（RhB）、四环素（TC）和盐酸左氧氟沙星（LEV））可被有效降解，光催化产氢速率达到10828.075 μmol g h，分别是COF-TpTt和BiOBr的12.4倍和8.5倍。此外，3,3',5,5'-四甲基联苯胺（TMB）氧化实验表明其具有优异的分子氧活化能力。此外，通过密度泛函理论（DFT）计算证明了S型异质结的电荷转移机制。在内建电场、能带弯曲和库仑力的影响下，电子和空穴被有效分离和转移。S型异质结的形成和多种自由基的产生确保了COF-TpTt@BiOBr-10%光催化体系的高氧化还原活性。本研究加深了我们对S型异质结电荷转移机制的深入理解，并为高效制氢提供了新途径。
