Retrospective suspect screening reveals previously ignored antibiotics, antifungal compounds, and metabolites in Bangladesh surface waters

Abstract

Densely populated countries in Asia, such as Bangladesh, are considered to be major contributors to the increased occurrence of global antimicrobial resistance (AMR). Several factors make low-and middle-income countries vulnerable to increased emergence and spread of AMR in the environment including limited regulations on antimicrobial drug use, high volume of antimicrobials used in human medicine and agricultural production, and poor wastewater management. Previous monitoring campaigns to investigate the presence of antibiotics in the aquatic environment have employed targeted analysis in which selected antibiotics are measured using liquid chromatography with tandem mass spectrometry (LC/MS/MS). However, this approach can miss several important contaminants that can contribute to the selective pressure that promotes maintenance and dissemination of antibiotic resistance genes (ARGs) in the environment. Nontarget analysis by suspect screening and reanalysis of stored digital data of previously ran samples can provide information on analytes that were formerly uncharacterized and may be chemicals of emerging concern (CECs). In this study, surface waters in both urban and rural sites in Bangladesh were collected and analyzed for the presence of antibiotic residues and other pharmaceuticals. Utilizing targeted analysis, the antibiotics with the highest concentrations detected were ciprofloxacin (1407 ng/L) and clarithromycin (909 ng/L). In addition, using high-resolution LC/MS/MS in the first ever application of retrospective analysis in samples from Bangladesh, additional antibiotics clindamycin, lincomycin, linezolid, metronidazole, moxifloxacin, nalidixic acid, and sulfapyridine were detected. Prevalence of amoxicillin transformation products in surface waters was also confirmed. In addition, medicinal and agricultural antifungal compounds were frequently found in Bangladeshi surface waters. This later finding – the near ubiquity of antifungal agents in environmental samples – is of particular concern, as it may be contributing to the alarming rise of multi-drug resistant fungal (e.g. Candida auris) disease recently seen in humans throughout the world.