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经典和生物膜废水处理中的沙坦类血压调节剂——浓度与代谢

Sartan blood pressure regulators in classical and biofilm wastewater treatment - Concentrations and metabolism.

作者信息

Li Rui, Liang Chuanzhou, Svendsen Sif B, Kisielius Vaidotas, Bester Kai

机构信息

Department of Environmental Science, Aarhus University, Frederiksborgvej 399, 4000, Roskilde, Denmark; WATEC - Centre for Water Technology, Aarhus University, Ny Munkegade 120, Aarhus 8000, Denmark.

Department of Environmental Science, Aarhus University, Frederiksborgvej 399, 4000, Roskilde, Denmark; School of Resources and Environmental Engineering, Wuhan University of Technology, Luoshi Road 122, Wuhan, 430070, China.

出版信息

Water Res. 2023 Feb 1;229:119352. doi: 10.1016/j.watres.2022.119352. Epub 2022 Nov 16.

DOI:10.1016/j.watres.2022.119352
PMID:36450176
Abstract

Sartans are a group of pharmaceuticals widely used to regulate blood pressure. Their concentration levels were monitored in 80 wastewater treatment plants (WWTP) in the Baltic Sea Region, reached from limit of detection up to 6 µg/L. The concentrations were significantly different in different countries, but consistent within the respective country. The degradation of sartans (losartan, valsartan, irbesartan) in moving bed biofilm reactors (MBBRs) that utilize biofilms grown on mobile carriers to treat wastewater was investigated for the first time, and compared with the degradation in a conventional activated sludge (CAS) treatment plant. The results showed the formation of six microbial transformation products (TPs) of losartan, four of valsartan, and four of irbesartan in biological wastewater treatment. Four of these metabolites have not been described in the literature before. Chemical structures were suggested and selected TPs were verified and quantified depending on availability of true standards. Valsartan acid was a common TP of losartan, valsartan, and irbesartan. Losartan and irbesartan also shared one TP: losartan/irbesartan TP335. Based on the mass balance analysis, losartan carboxylic acid is the main TP of losartan, and valsartan acid is the main TP of valsartan during the biotransformation process. For irbesartan, TP447 is likely to be the main TP, as its peak areas were two orders of magnitude higher than those of all the other detected TPs of this compound. The effects of adapting biofilms to different biological oxygen demand (BOD) loading on the degradation of sartans as well as the formation of their TPs were investigated. Compared to feeding a poor substrate (pure effluent wastewater from a CAS), feeding with richer substrate (1/3 raw and 2/3 effluent wastewater) promoted the metabolism of most compounds (co-metabolization). However, the addition of raw wastewater inhibited some metabolic pathways of other compounds, such as from losartan/irbesartan to TP335 (competitive inhibition). The formation of irbesartan TP447 did not change with or without raw wastewater. Finally, the sartans and their TPs were investigated in a full-scale CAS wastewater treatment plant (WWTP). The removal of losartan, valsartan, and irbesartan ranged from 3.0 % to 72% and some of the transformation products (TPs) from human metabolism were also removed in the WWTP. However, some of the sartan TPs, i.e., valsartan acid, losartan carboxylic acid, irbesartan TP443 and losartan TP453, were formed in the WWTP. Relative high amounts of especially losartan carboxylic acid, which was detected with concentrations up to 2.27 µg/L were found in the effluent.

摘要

沙坦类药物是一类广泛用于调节血压的药物。对波罗的海地区80家污水处理厂(WWTP)中的沙坦类药物浓度水平进行了监测,其浓度范围从检测限到6微克/升。不同国家的浓度存在显著差异,但在各自国家内具有一致性。首次研究了利用移动载体上生长的生物膜处理废水的移动床生物膜反应器(MBBR)中沙坦类药物(氯沙坦、缬沙坦、厄贝沙坦)的降解情况,并与传统活性污泥(CAS)处理厂中的降解情况进行了比较。结果表明,在生物废水处理过程中,氯沙坦形成了6种微生物转化产物(TPs),缬沙坦形成了4种,厄贝沙坦形成了4种。其中有4种代谢物此前在文献中未被描述。根据真实标准品的可得性,提出了化学结构,并对选定的TPs进行了验证和定量。缬沙坦酸是氯沙坦、缬沙坦和厄贝沙坦的常见TP。氯沙坦和厄贝沙坦还共享一种TP:氯沙坦/厄贝沙坦TP335。基于质量平衡分析,氯沙坦羧酸是氯沙坦生物转化过程中的主要TP,缬沙坦酸是缬沙坦的主要TP。对于厄贝沙坦,TP447可能是主要TP,因为其峰面积比该化合物所有其他检测到的TPs高两个数量级。研究了使生物膜适应不同生物需氧量(BOD)负荷对沙坦类药物降解及其TPs形成的影响。与投喂劣质底物(CAS的纯出水废水)相比,投喂优质底物(1/3原水和2/3出水废水)促进了大多数化合物的代谢(共代谢)。然而,原水的添加抑制了其他化合物的一些代谢途径,例如从氯沙坦/厄贝沙坦到TP335的代谢途径(竞争性抑制)。有无原水时厄贝沙坦TP447的形成均未改变。最后,在一座全尺寸CAS污水处理厂(WWTP)中对沙坦类药物及其TPs进行了研究。氯沙坦、缬沙坦和厄贝沙坦的去除率在3.0%至72%之间,污水处理厂中还去除了一些来自人体代谢的转化产物(TPs)。然而,污水处理厂中形成了一些沙坦类TPs,即缬沙坦酸、氯沙坦羧酸、厄贝沙坦TP443和氯沙坦TP453。在出水水中发现了相对大量的氯沙坦羧酸,其检测浓度高达2.27微克/升。

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