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Removal of antibiotics, antibiotic-resistant bacteria and their associated genes by graphene-based TiO2 composite photocatalysts under solar radiation in urban wastewaters
Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2017-11-10 , DOI: 10.1016/j.apcatb.2017.11.020
Popi Karaolia , Irene Michael-Kordatou , Evroula Hapeshi , Catherine Drosou , Yannis Bertakis , Dimitris Christofilos , Gerasimos S. Armatas , Labrini Sygellou , Thomas Schwartz , Nikolaos P. Xekoukoulotakis , Despo Fatta-Kassinos

The present work investigated: (i) the removal of the antibiotics sulfamethoxazole (SMX), erythromycin (ERY) and clarithromycin (CLA); (ii) the inactivation of the total and antibiotic-resistant E. coli along with their regrowth potential after treatment; (iii) the removal of the total genomic DNA content; and (iv) the removal of selected antibiotic resistance genes (ARGs), namely sul1, ampC, ermB, mecA, as well as species-specific sequences, namely ecfX for Pseudomonas aeruginosa and enterococci-specific 23S rRNA, by graphene-based TiO2 composite photocatalysts under solar radiation, in real urban wastewaters. TiO2-reduced graphene oxide (TiO2-rGO) composite photocatalysts were synthesized by two ex-situ synthesis methods, namely hydrothermal (HD) treatment and photocatalytic (PH) treatment, starting from graphene oxide and Aeroxide P25 TiO2, and were characterized with various techniques, such as XRD, FT-IR, Raman, XPS, SEM and surface area (BET) analyses. The potential of the synthesized TiO2-rGO composites for the removal of the abovementioned antibiotic-related microcontaminants was compared to the efficiency shown by pristine Aeroxide P25 TiO2 under simulated solar radiation, in real urban wastewater effluents treated by a membrane bioreactor. The results showed that TiO2-rGO-PH was more efficient in the photocatalytic degradation of ERY (84 ± 2%) and CLA (86 ± 5%), while degradation of SMX (87 ± 4%) was found to be slightly higher with Aeroxide P25 TiO2. It was also demonstrated that more than 180 min of treatment were satisfactory for the complete inactivation and complete absence of post-treatment regrowth of E. coli bacteria (<LOD) even 24 h after the end of the treatment, for all examined photocatalytic materials. The least amount of regrowth at all experimental times was observed in the presence of TiO2-rGO-HD. Moreover, the synthesized graphene-based photocatalysts successfully removed ampC and significantly reduced ecfX abundance of Pseudomonas aeruginosa, but sul1, ermB and 23S rRNA for enterococci sequences were found to be persistent throughout treatment with all catalyst types. Finally, the total DNA concentration remained stable throughout the photocatalytic treatment (4.2–4.8 ng μL−1), indicating the high total genomic DNA stability in treated wastewater and its resistance to photocatalytic treatment.



中文翻译:

太阳辐射下石墨烯基TiO 2复合光催化剂去除抗生素,抗药性细菌及其相关基因

本工作研究:(i)去除抗生素磺胺甲恶唑(SMX),红霉素(ERY)和克拉霉素(CLA);(ii)治疗后使总的和抗药性的大肠杆菌灭活,以及它们的再生潜力;(iii)去除总基因组DNA含量;(iv)去除选定的抗生素抗性基因(ARG),即sul 1,amp C,erm B,mec A,以及物种特异性序列,即铜绿假单胞菌和肠球菌特异性23S rRNA的ecf X ,实际城市废水中在太阳辐射下的石墨烯基TiO 2复合光催化剂。二氧化钛2-减少石墨烯氧化钛(TiO 2 -rGO)复合光通过两种合成易地合成方法,即水热(HD)治疗和光催化(PH)处理,从氧化石墨烯和P25的Aeroxide开始的TiO 2,和进行了表征与各种XRD,FT-IR,拉曼,XPS,SEM和表面积(BET)分析等技术。在膜生物反应器处理的实际城市废水中,将合成的TiO 2 -rGO复合材料去除上述抗生素相关的微污染物的潜力与原始Aeroxide P25 TiO 2在模拟太阳辐射下显示的效率进行了比较。结果表明,TiO 2-rGO-PH在ERY(84±2%)和CLA(86±5%)的光催化降解方面更有效,而Aeroxide P25 TiO 2的SMX(87±4%)降解则稍高。还证明对于所有检查的光催化材料,即使在处理结束后24小时,超过180分钟的处理对于大肠杆菌的完全灭活和处理后再生长的完全不满意(<LOD)也是令人满意的。在存在TiO 2 -rGO-HD的情况下,在所有实验时间观察到最少的再生长。此外,合成的石墨烯基光催化剂成功去除了amp C,并显着降低了Ecf X丰度。铜绿假单胞菌Pseudomonas aeruginosa),但肠球菌序列的sul 1,erm B和23S rRNA在使用所有催化剂类型的整个治疗过程中均持续存在。最后,在整个光催化处理过程中,总DNA浓度保持稳定(4.2–4.8 ngμL -1),表明处理过的废水中的总基因组DNA稳定性很高,并且对光催化处理具有抗性。

更新日期:2017-11-10
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