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通过电子给体同步构建多孔分子内D-A共轭聚合物用于高效光催化去污

Synchronous construction of a porous intramolecular D-A conjugated polymer via electron donors for superior photocatalytic decontamination.

作者信息

Wang Zhongquan, Zheng Xiaoshan, Chen Ping, Li Daguang, Zhang Qianxin, Liu Haijin, Zhong Jiapeng, Lv Wenying, Liu Guoguang

机构信息

School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China.

School of Environment, Tsinghua University, Beijing 100084, China.

出版信息

J Hazard Mater. 2022 Feb 15;424(Pt B):127379. doi: 10.1016/j.jhazmat.2021.127379. Epub 2021 Sep 29.

DOI:10.1016/j.jhazmat.2021.127379
PMID:34655871
Abstract

The development of conjugated polymers with intramolecular donor-acceptor (D-A) units has the capacity to enhance the photocatalytic performance of carbon nitride (g-CN) for the removal of antibiotics from ambient ecosystems. This strategy addresses the challenge of narrowing the band gap of g-CN while maintaining its high LUMO position. For this study, we introduced the above donor units into g-CN to construct intramolecular D-A structures through the copolymerization of dicyandiamide with creatinine, which strategically extended light absorption into the green region and expedited photoelectron separation. The introduction of electron donor blocks kept the LUMO distributed on the melem, which maintained the high LUMO energy level of the copolymer with the potential to generate oxygen radicals. The as-prepared porous D-A conjugated polymer enhanced the photocatalytic degradation of sulfisoxazole with kinetic constants 5.6 times higher than that of g-CN under blue light and 15.3 times higher under green light. Furthermore, we surveyed the degradation mechanism including the effective active species and degradation pathways. This study offers a new perspective for the synchronous construction of a porous intramolecular D-A conjugated polymer to enhance water treatment and environmental remediation capacities.

摘要

具有分子内供体-受体(D-A)单元的共轭聚合物的开发,有能力增强氮化碳(g-CN)从周围生态系统中去除抗生素的光催化性能。该策略解决了在保持g-CN高LUMO位置的同时缩小其带隙的挑战。在本研究中,我们将上述供体单元引入g-CN,通过双氰胺与肌酸酐的共聚构建分子内D-A结构,从而将光吸收战略性地扩展到绿色区域并加速光电子分离。电子供体嵌段的引入使LUMO分布在蜜勒胺上,这保持了共聚物的高LUMO能级,使其有产生氧自由基的潜力。所制备的多孔D-A共轭聚合物增强了磺胺异恶唑的光催化降解,其动力学常数在蓝光下比g-CN高5.6倍,在绿光下高15.3倍。此外,我们研究了包括有效活性物种和降解途径在内的降解机制。本研究为同步构建多孔分子内D-A共轭聚合物以提高水处理和环境修复能力提供了新的视角。

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