Department of Environmental Science, Exposure and Effects Unit, Science for Life Laboratory, Stockholm University, Stockholm 106 91, Sweden.
Immunobiology, Nutrition and Toxicology Unit, Infectious Diseases Division, International Centre for Diarrhoeal Disease Research, Bangladesh (icddr,b), Dhaka 1212, Bangladesh.
Environ Sci Technol. 2023 May 2;57(17):6808-6824. doi: 10.1021/acs.est.2c08200. Epub 2023 Apr 21.
Nontarget mass spectrometry has great potential to reveal patterns of water contamination globally through community science, but few studies are conducted in low-income countries, nor with open-source workflows, and few datasets are FAIR (Findable, Accessible, Interoperable, Reusable). Water was collected from urban and rural rivers around Dhaka, Bangladesh, and analyzed by liquid chromatography high-resolution mass spectrometry in four ionization modes (electrospray ionization ±, atmospheric pressure chemical ionization ±) with data-independent MS2 acquisition. The acquisition strategy was complementary: 19,427 and 7365 features were unique to ESI and APCI, respectively. The complexity of water pollution was revealed by >26,000 unique molecular features resolved by MS-DIAL, among which >20,000 correlated with urban sources in Dhaka. A major wastewater treatment plant was not a dominant pollution source, consistent with major contributions from uncontrolled urban drainage, a result that encourages development of further wastewater infrastructures. Matching of deconvoluted MS2 spectra to public libraries resulted in 62 confident annotations (, Level 1-2a) and allowed semiquantification of 42 analytes including pharmaceuticals, pesticides, and personal care products. structure prediction for the top 100 unknown molecular features associated with an urban source allowed 15 additional chemicals of anthropogenic origin to be annotated (, Level 3). The authentic MS2 spectra were uploaded to MassBank Europe, mass spectral data were openly shared on the MassIVE repository, a tool (, MASST) that could be used for community science environmental surveillance was demonstrated, and current limitations were discussed.
非靶向质谱分析通过社区科学具有揭示全球水污染模式的巨大潜力,但在低收入国家、使用开源工作流程的研究很少,并且很少有数据集符合 FAIR(可查找、可访问、可互操作、可重复使用)标准。本研究从孟加拉国达卡市的城市和农村河流中采集水样,采用四种电离模式(电喷雾电离 ±、大气压化学电离 ±)的液相色谱高分辨质谱法进行分析,并进行数据非依赖 MS2 采集。该采集策略是互补的:ESI 和 APCI 分别有 19427 个和 7365 个特征是独特的。通过 MS-DIAL 解析出超过 26000 个独特的分子特征,揭示了水污染的复杂性,其中超过 20000 个特征与达卡的城市源相关。一个主要的污水处理厂并不是主要的污染源,这与不受控制的城市排水有很大关系,这一结果鼓励进一步开发废水基础设施。将解卷积的 MS2 谱图与公共库进行匹配,得到 62 个可靠注释(,Level 1-2a),并允许对 42 种分析物进行半定量分析,包括药物、农药和个人护理产品。与城市源相关的前 100 个未知分子特征的结构预测允许注释 15 种额外的人为来源的化学物质(,Level 3)。真实的 MS2 谱图已上传至 MassBank Europe,质谱数据已在 MassIVE 存储库中公开共享,展示了可用于社区科学环境监测的工具(,MASST),并讨论了当前的限制。