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Degradation of anticancer drug capecitabine in aquatic media by three advanced oxidation processes: Mechanisms, toxicity changes and energy cost evaluation
Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-10-26 , DOI: 10.1016/j.cej.2020.127489
Shaoyu Tang , Lei Xu , Xiaolong Yu , Shuona Chen , Huanyong Li , Ying Huang , Junfeng Niu

Degradation of capecitabine was conducted using electrochemical oxidation, UV/H2O2 oxidation, and ozonation. Capecitabine was efficiently degraded by three advanced oxidation processes. The degradation rates of capecitabine achieved approximately 99.0% after 4 min of ozonation, 12 min of electrochemical oxidation, and 30 min of UV/H2O2 oxidation. The mineralization rate obtained was merely 10.3% for ozonation at 60 min, compared to 91.7% for electrochemical oxidation and 55.3% for UV/H2O2 oxidation. Capecitabine was degraded by oxidation, defluorination, hydrogenation, hydrolysis, ring and bond cleavage. Thus, multiple intermediates were generated during the degradation process, such as F-, formic acid, acetic acid, oxalic acid, and other intermediate metabolites with lager molecules. A total of eighteen metabolites, except for F- and carboxylic acids, were identified by QTOF-HRMS, where six of them could only be detected by the electrochemical oxidation process, two of them were by the UV/H2O2 oxidation process, and one of them by the ozonation process. Electrochemical oxidation was the only process that could achieve over 90% removal of cytotoxicity and genotoxicity, and the metabolites were non-genotoxic after 60 min of reaction. The number of live cells decreased with the increasing reaction time in ozonation, demonstrating the higher toxicity of the intermediates in ozonation. Energy cost evaluation results suggested that the lowest energy consumption was achieved at 1.8 kWh/m3 for 90% of capecitabine degradation with the O3 dosage of 250 mg/h. Energy consumptions for 50% removal of cytotoxicity were 21.3 and 6.3 kWh/m3 in electrochemical oxidation and UV/H2O2 oxidation, respectively. The highest energy cost for 50% of genotoxicity removal was observed in electrochemical oxidation, while ozonation was identified as the most cost-effective process.



中文翻译:

通过三种先进的氧化过程降解水介质中的抗癌药物卡培他滨:机理,毒性变化和能源成本评估

卡培他滨的降解使用电化学氧化,UV / H 2 O 2氧化和臭氧化进行。卡培他滨可通过三种高级氧化过程有效降解。臭氧化4分钟,电化学氧化12分钟和UV / H 2 O 2氧化30分钟后,卡培他滨的降解率达到约99.0%。对于60分钟的臭氧化,获得的矿化率仅为10.3%,而电化学氧化的矿化率为91.7%,UV / H 2 O 2的矿化率为55.3%氧化。卡培他滨通过氧化,脱氟,氢化,水解,环和键裂解而降解。因此,在降解过程,如F生成的多个中间体- ,甲酸,乙酸,草酸,和与啤酒分子其它中间代谢物。共有18种代谢物,除了˚F -和羧酸,通过QTOF-HRMS,其中六他们只能通过电化学氧化过程来检测确定,其中两人通过UV / H 2 ö 2氧化过程,其中之一是通过臭氧化过程。电化学氧化是唯一可以超过90%去除细胞毒性和遗传毒性的过程,并且代谢产物在反应60分钟后没有遗传毒性。活细胞的数目随着臭氧化反应时间的增加而减少,这表明中间体在臭氧化中的毒性更高。能源成本评估结果表明,对于90%的卡培他滨降解,当O 3剂量为250 mg / h时,最低能耗为1.8 kWh / m 3。在电化学氧化和UV / H 2 O 2中,去除细胞毒性50%的能量消耗分别为21.3和6.3 kWh / m 3氧化。在电化学氧化中,观察到了50%的遗传毒性去除所需的最高能源成本,而臭氧氧化被认为是最具成本效益的过程。

更新日期:2020-10-30
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