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介孔 g-CN 负载碳量子点的简便合成及其对氟喹诺酮类抗生素的协同吸附和可见光光降解

Facile synthesis of carbon quantum dots loaded with mesoporous g-CN for synergistic absorption and visible light photodegradation of fluoroquinolone antibiotics.

机构信息

School of Environmental Science and Engineering, Institute of Environmental Health and Pollution Control, Guangdong University of Technology, Guangzhou, 510006, China.

出版信息

Dalton Trans. 2018 Jan 23;47(4):1284-1293. doi: 10.1039/c7dt04360k.

DOI:10.1039/c7dt04360k
PMID:29299582
Abstract

The development of facile and efficient synthetic approaches of carbon quantum dots loaded with mesoporous g-CN (mpg-CN/CQDs) is of critical urgency. Here, a facile strategy was developed to synthesize the mpg-CN/CQDs by using calcinations of the mixture of CQDs, cyanamide, and silica colloid. The obtained composite still retained a considerable total surface area, which could offer a larger population of adsorption sites; therefore enhance the capacity for the adsorption of fluoroquinolones antibiotics (FQs). Under visible light irradiation, mpg-CN/CQDs demonstrated a higher photocatalytic activity for FQs degradation than did bulk g-CN or mpg-CN. This enhancement might have been ascribed to the high surface area of the mpg-CN, unique up-converted photoluminescence (PL) properties, and the efficient charge separation of the CQDs. The eradication of FQs followed the Langmuir-Hinshelwood (L-H) kinetic degradation model and absorption pseudo-second-order kinetic model, indicating that surface reactions and chemical sorption played significant roles during the photocatalysis process. The results of electron spin resonance (ESR) technology and reactive species (RSs) scavenging experiments revealed that the superoxide anion radical (O˙) and photo-hole (h) were the primarily active species that initiated the degradation of FQs. Based on the identification of intermediates and the prediction of reactive sites, the degradation pathways of ofloxacin (OFX) were proposed. A residual antibiotic activity experiment revealed that mpg-CN/CQDs provided very desirable performance for the reduction of antibiotic activity.

摘要

开发简便高效的负载介孔 g-CN(mpg-CN/CQDs)的碳量子点合成方法至关重要。本文采用碳量子点、氰胺和硅胶胶体混合物煅烧的方法,简便地合成了 mpg-CN/CQDs。所得复合材料仍保留相当大的总表面积,可提供更多的吸附位,从而增强对氟喹诺酮类抗生素(FQs)的吸附能力。在可见光照射下,mpg-CN/CQDs 对 FQs 的光催化降解活性高于体相 g-CN 或 mpg-CN。这种增强可能归因于 mpg-CN 的高比表面积、独特的上转换光致发光(PL)特性以及 CQDs 的有效电荷分离。FQs 的消除遵循 Langmuir-Hinshelwood(L-H)动力学降解模型和吸附准二级动力学模型,表明在光催化过程中表面反应和化学吸附起重要作用。电子自旋共振(ESR)技术和活性物质(RSs)清除实验的结果表明,超氧阴离子自由基(O˙)和光穴(h)是引发 FQs 降解的主要活性物质。基于中间产物的鉴定和反应位点的预测,提出了氧氟沙星(OFX)的降解途径。残留抗生素活性实验表明,mpg-CN/CQDs 对降低抗生素活性具有良好的性能。

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