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Photocatalytic degradation of fluoroquinolone antibiotics using ordered mesoporous g-C3N4 under simulated sunlight irradiation: Kinetics, mechanism, and antibacterial activity elimination
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2018-01-11 , DOI: 10.1016/j.apcatb.2018.01.024
Fengliang Wang , Yiping Feng , Ping Chen , Yingfei Wang , Yuehan Su , Qianxin Zhang , Yongqin Zeng , Zhijie Xie , Haijin Liu , Yang Liu , Wenying Lv , Guoguang Liu

The occurrence of fluoroquinolones (FQs) in the ambient environment has raised serious concerns. In this study, the photocatalytic degradation kinetics and mechanism of ciprofloxacin (CIP) was investigated in ordered mesoporous g-C3N4 (ompg-C3N4). Under simulated sunlight irradiation, ompg-C3N4 exhibited a 2.9 fold more rapid reaction for CIP degradation than bulk g-C3N4. This enhancement may be attributed to the large specific surface area and effective charge separation of ompg-C3N4. The eradication of CIP followed the Langmuir–Hinshelwood (L–H) kinetics model, and surface reactions played a significant role during the photocatalysis process. Further study of reactive species (RSs) by both ESR technology and RSs scavenging experiments revealed that the superoxide anion radical (O2) and photohole (h+) were primarily responsible for the degradation of CIP. Based on the identification of intermediates using liquid chromatography with tandem mass spectrometry (HPLC-MS/MS), and the prediction of reactive sites via Frontier Electron Densities (FEDs), the degradation pathways of CIP were proposed. A comparison of the degradation among FQs revealed that the piperazine moiety showed a dramatic effect on the degradation of FQs during the photocatalysis process. A residual antibiotic activity experiment revealed that ompg-C3N4 provided a very desirable performance for the reduction of antibiotic activity. The sufficient photocatalytic degradation of CIP in ambient water revealed that a sunlight-driven ompg-C3N4 photocatalytic process may be efficiently applied for the remediation of CIP contaminated natural waters.



中文翻译:

在模拟的阳光照射下使用有序介孔gC 3 N 4光催化降解氟喹诺酮类抗生素:动力学,机理和消除抗菌活性

周围环境中氟喹诺酮类(FQs)的出现引起了人们的严重关注。在这项研究中,在有序介孔gC 3 N 4(ompg-C 3 N 4)中研究了环丙沙星(CIP)的光催化降解动力学和机理。在模拟的阳光照射下,ompg-C 3 N 4的CIP降解反应比块状gC 3 N 4快2.9倍。这种增强可能归因于ompg-C 3 N 4的较大的比表面积和有效的电荷分离。CIP的消除遵循Langmuir-Hinshelwood(L-H)动力学模型,并且表面反应在光催化过程中起着重要作用。通过既ESR技术和RSS清除实验反应性物质(RS)的的进一步研究显示,超氧阴离子自由基(O 2 - )和光空穴(H +)是导致CIP降级的主要原因。基于液相色谱-串联质谱(HPLC-MS / MS)鉴定中间体,并通过前沿电子密度(FEDs)预测反应位点,提出了CIP的降解途径。对FQ之间降解的比较表明,哌嗪部分在光催化过程中对FQ降解表现出显着影响。残留的抗生素活性实验表明,ompg-C 3 N 4为降低抗生素活性提供了非常理想的性能。CIP在环境水中的充分光催化降解表明,阳光驱动的ompg-C 3 N 4 光催化过程可以有效地应用于CIP污染的天然水的修复。

更新日期:2018-01-11
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