Ciccarelli Davide, Christopher Braddock D, Surman Andrew J, Arenas Blanca Ivonne Vergara, Salal Tara, Marczylo Tim, Vineis Paolo, Barron Leon P
Environmental Research Group, MRC Centre for Environment and Health, School of Public Health, Imperial College London, 86 Wood Lane, London W12 0BZ, UK; NIHR-HPRU Chemical and Radiation Threats and Hazards, NIHR-HPRU Environmental Exposures and Health, MRC Centre for Environment and Health, School of Public Health, Imperial College London, 86 Wood Lane, London W12 0BZ, UK.
Department of Chemistry, Imperial College London, 82 Wood Lane, London W12 7TA, UK.
J Hazard Mater. 2023 Apr 15;448:130906. doi: 10.1016/j.jhazmat.2023.130906. Epub 2023 Jan 31.
A novel analytical workflow for suspect screening of organic acidic contaminants in drinking water is presented, featuring selective extraction by silica-based strong anion-exchange solid-phase extraction, mixed-mode liquid chromatography-high resolution accurate mass spectrometry (LC-HRMS), peak detection, feature reduction and compound identification. The novel use of an ammonium bicarbonate-based elution solvent extended strong anion-exchange solid-phase extraction applicability to LC-HRMS of strong acids. This approach performed with consistently higher recovery and repeatability (88 ± 7 % at 500 ng L), improved selectivity and lower matrix interference (mean = 12 %) over a generic mixed-mode weak anion exchange SPE method. In addition, a novel filter for reducing full-scan features from fulvic and humic acids was successfully introduced, reducing workload and potential for false positives. The workflow was then applied to 10 London municipal drinking water samples, revealing the presence of 22 confirmed and 37 tentatively identified substances. Several poorly investigated and potentially harmful compounds were found which included halogenated hydroxy-cyclopentene-diones and dibromomethanesulfonic acid. Some of these compounds have been reported as mutagenic in test systems and thus their presence here requires further investigation. Overall, this approach demonstrated that employing selective extraction improved detection and helped shortlist suspects and potentially toxic chemical contaminants with higher confidence.
本文介绍了一种用于饮用水中有机酸性污染物可疑物筛查的新型分析工作流程，其特点包括基于硅胶的强阴离子交换固相萃取进行选择性萃取、混合模式液相色谱-高分辨率精确质量质谱（LC-HRMS）、峰检测、特征约简和化合物鉴定。基于碳酸氢铵的洗脱溶剂的新应用将强阴离子交换固相萃取的适用性扩展到强酸的LC-HRMS分析。与通用的混合模式弱阴离子交换固相萃取方法相比，该方法具有更高的回收率和重复性（500 ng/L时为88±7%）、更好的选择性和更低的基质干扰（平均值=12%）。此外，成功引入了一种用于减少富里酸和腐殖酸全扫描特征的新型过滤器，减少了工作量和假阳性的可能性。然后将该工作流程应用于10个伦敦市饮用水样本，发现了22种已确认和37种初步鉴定的物质。发现了几种研究较少且可能有害的化合物，包括卤代羟基环戊烯二酮和二溴甲磺酸。其中一些化合物在测试系统中已被报道具有致突变性，因此它们在此处的存在需要进一步研究。总体而言，该方法表明采用选择性萃取可提高检测能力，并有助于更有信心地筛选可疑物和潜在有毒化学污染物。
