Pub Date : 2026-10-15DOI: 10.1021/acs.jafc.6c09760
Wen Hao,Xueyan Cui,Lin Cai,Yichuan Cao,Guozhen Fang,Shuo Wang
Abstract Antibiotic contamination poses environmental risks and requires efficient degradation technologies. Herein, a Z-scheme heterostructured photocatalyst (CMCN/Co3O4-ZIF-8) was constructed by thermally coupling precursor-modified graphitic carbon nitride (CMCN) with metal–organic framework (MOF) derivative (Co3O4-ZIF-8) for tetracycline degradation. Temperature-regulated pyrolysis of ZnCo-MOF afforded Co3O4-ZIF-8 with in situ-formed Co3O4 active sites and a porous framework. CMCN/Co3O4-ZIF-8 heterointerface promoted charge separation and migration via interfacial electric field and energy gradient, enabling Z-scheme charge-transfer pathway that retained highly reductive electrons on Co3O4-ZIF-8 and strongly oxidative holes on CMCN. The Co2+/Co3+ redox cycle in Co3O4-ZIF-8 further facilitated interfacial electron transfer and O2 activation. Superoxide radicals and oxidative holes participated in tetracycline degradation, achieving a degradation efficiency of 86.88%. LC-MS analysis revealed major tetracycline degradation pathways, and toxicity evaluation indicated reduced toxicity of most intermediates. This study guided catalyst design by integrating in situ active site formation and Z-scheme charge-transfer pathway for antibiotic removal.
抗生素污染具有环境风险,需要高效的降解技术。本文采用前驱体修饰的石墨氮化碳(CMCN)与金属有机骨架(MOF)衍生物(Co3O4-ZIF-8)热偶联的方法,构建了用于四环素降解的z型异质结构光催化剂(CMCN/Co3O4-ZIF-8)。ZnCo-MOF的温度调节热解使Co3O4- zif -8具有原位形成的Co3O4活性位点和多孔骨架。CMCN/Co3O4-ZIF-8异质界面通过界面电场和能量梯度促进电荷分离和迁移,实现了在Co3O4-ZIF-8上保留高还原电子和CMCN上保留强氧化空穴的Z-scheme电荷转移途径。Co3O4-ZIF-8中的Co2+/Co3+氧化还原循环进一步促进了界面电子转移和O2活化。超氧自由基和氧化空穴参与四环素的降解,降解效率为86.88%。LC-MS分析揭示了主要的四环素降解途径,毒性评价表明大多数中间体毒性降低。本研究通过整合原位活性位点形成和Z-scheme电荷转移途径来指导抗生素去除的催化剂设计。
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