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具有氧空位和 N 掺杂 CQDs 修饰的 BiOBr 纳米复合材料的可见光驱动光催化降解氧氟沙星:增强的光降解性能和机制。

Visible-light-driven photocatalytic degradation of ofloxacin by BiOBr nanocomposite modified with oxygen vacancies and N-doped CQDs: Enhanced photodegradation performance and mechanism.

机构信息

Beijing Key Laboratory for Source Control Technology of Water Pollution, Engineering Research Center for Water Pollution Source Control and Eco-remediation, Beijing Forestry University, Beijing, 100083, China.

Beijing Key Laboratory for Source Control Technology of Water Pollution, Engineering Research Center for Water Pollution Source Control and Eco-remediation, Beijing Forestry University, Beijing, 100083, China.

出版信息

Chemosphere. 2022 Nov;307(Pt 3):135976. doi: 10.1016/j.chemosphere.2022.135976. Epub 2022 Aug 6.

Abstract

The rapid recombination of photogenerated carriers and weak light absorption capacity are two major challenges for bismuth-based photocatalysts. Here, N-CQDs/BiOBr micro-flower photocatalysts with the visible-light activity were fabricated through the ethylene glycol solvothermal method for the first time, and oxygen vacancies (OVs) and N-doped carbon quantum dots (N-CQDs) were simultaneously introduced on the surface of BiOBr. OVs were introduced to form defective BiOBr (BiOBr). N-CQDs and BiOBr formed a strong binding effect. Then, the composition, morphology, crystal structure and photoelectric property of photocatalysts were studied, and the mechanism and pathway of ofloxacin (OFL) photodegradation were studied. N-CQDs/BiOBr-4 was a micro-flower composed of nanosheets with a thickness of about 60 nm, this structure produced multiple light reflections. Photoelectrochemical analysis confirmed that the synergistic effect of OVs and N-CQDs significantly promoted the electron-hole separation (3 times vs BiOBr) and enhanced the light absorption range (Eg = 2.96 eV vs 3.24 eV). Meanwhile, the removal rate of OFL by N-CQDs/BiOBr-4 was 6 times higher than that by BiOBr (K of N-CQDs/BiOBr-4 was 32 times higher than that of BiOBr). Electron spin resonances analysis and radical quenching experiments showed that ·O and h played dominant roles in the OFL photodegradation system, and their contribution rates were 89.84% and 70.31%, respectively. There were main degradation pathways for OFL, including oxidation, dealkylation, hydroxylation and decarboxylation. This study explored the synergistic and complementary effects between OVs and N-CQDs, and provided a promising strategy for the photodegradation of toxic antibiotics by visible-light-driven photocatalysts.

摘要

光生载流子的快速复合和弱光吸收能力是铋基光催化剂面临的两大挑战。本研究首次通过乙二醇溶剂热法制备了具有可见光活性的 N-CQDs/BiOBr 微花光催化剂,同时在 BiOBr 表面引入氧空位(OVs)和 N 掺杂碳量子点(N-CQDs)。OVs 的引入形成了缺陷型 BiOBr(BiOBr)。N-CQDs 和 BiOBr 形成了强结合效应。然后,研究了光催化剂的组成、形貌、晶体结构和光电性能,并研究了氧氟沙星(OFL)光降解的机制和途径。N-CQDs/BiOBr-4 是由厚度约为 60nm 的纳米片组成的微花,这种结构产生了多次光反射。光电化学分析证实,OVs 和 N-CQDs 的协同作用显著促进了电子-空穴分离(比 BiOBr 提高了 3 倍),并增强了光吸收范围(Eg=2.96eV 比 3.24eV)。同时,N-CQDs/BiOBr-4 对 OFL 的去除率比 BiOBr 高 6 倍(N-CQDs/BiOBr-4 的 K 比 BiOBr 高 32 倍)。电子自旋共振分析和自由基淬灭实验表明,·O 和 h 在 OFL 光降解体系中起主导作用,其贡献率分别为 89.84%和 70.31%。OFL 有主要的降解途径,包括氧化、脱烷基、羟化和脱羧。本研究探讨了 OVs 和 N-CQDs 之间的协同互补效应,为可见光驱动光催化剂降解有毒抗生素提供了一种有前途的策略。

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