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通过π-π相互作用实现强界面电荷转移的苝二酰亚胺/铁酞菁 Z 型异质结:盐酸四环素的高效光催化降解。

Perylene diimide/iron phthalocyanine Z-scheme heterojunction with strong interfacial charge transfer through π-π interaction: Efficient photocatalytic degradation of tetracycline hydrochloride.

机构信息

School of Chemistry and Chemical Engineering, Jiangxi University of Science and Technology, Ganzhou, 341000, Jiangxi, China.

School of Pharmaceutical Sciences, Gannan Medical University, Ganzhou, 341000, Jiangxi, China.

出版信息

Chemosphere. 2023 Jul;329:138617. doi: 10.1016/j.chemosphere.2023.138617. Epub 2023 Apr 8.

Abstract

The development of an all-organic Z-scheme heterojunction photocatalyst with the matched band structure, efficient electron transfer and excellent photocatalytic performance is valuable for a sustainable future. A novel perylene diimide/phthalocyanine iron (PDI/FePc) heterojunctions with strong π-π interaction were synthesized by a self-assembled method, which exhibited strong visible-light-driven photocatalytic degradation activities of tetracycline hydrochloride (TC). The TC removal rate over PDI/FePc was achieved three times and 87.5 times higher than that of PDI and FePc. PDI/FePc (131.1 mv·dec) presented a lower Taffel slope than that of PDI (228.6 mv·dec) for the oxidation. This may be due to the strong π-π interactions between PDI and FePc, which can reduce the layer spacing of the supramolecular structure and facilitate the separation and transfer of photogenerated carriers in the built-in electric field. In addition, radical quenching tests revealed that superoxide radicals (•O) acted as a dominant role in photocatalytic oxidation. An increscent specific surface area of PDI decorated by FePc also gave the rapid pathway for charge transfer and enhanced the adsorption ability. This provides a new idea for the formation of heterojunction to improve the photocatalytic activity of organic supramolecular materials.

摘要

开发具有匹配能带结构、高效电子转移和优异光催化性能的全有机 Z 型异质结光催化剂对于可持续的未来是有价值的。通过自组装方法合成了具有强π-π相互作用的新型苝二酰亚胺/酞菁铁(PDI/FePc)异质结,其表现出很强的可见光驱动的盐酸四环素(TC)光催化降解活性。PDI/FePc 的 TC 去除率比 PDI 和 FePc 分别高出三倍和 87.5 倍。PDI/FePc(131.1 mv·dec)的 Taffel 斜率比 PDI(228.6 mv·dec)低,这可能是由于 PDI 和 FePc 之间存在强的π-π相互作用,这可以减小超分子结构的层间距,并促进内置电场中光生载流子的分离和转移。此外,自由基猝灭实验表明,超氧自由基(•O)在光催化氧化中起主要作用。FePc 修饰的 PDI 的比表面积增大也为电荷转移提供了快速途径,并增强了吸附能力。这为形成异质结以提高有机超分子材料的光催化活性提供了新的思路。

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