Exposure and Biomonitoring Division, Environmental Health Science and Research Bureau, Environmental and Radiation Health Sciences Directorate, Healthy Environments and Consumer Safety Branch, Health Canada, AL: 2203 B, 251 Sir Frederick Banting Driveway, Ottawa, Ontario, K1A 0K9, Canada.
Exposure and Biomonitoring Division, Environmental Health Science and Research Bureau, Environmental and Radiation Health Sciences Directorate, Healthy Environments and Consumer Safety Branch, Health Canada, AL: 2203 B, 251 Sir Frederick Banting Driveway, Ottawa, Ontario, K1A 0K9, Canada.
Chemosphere. 2024 Sep;363:142754. doi: 10.1016/j.chemosphere.2024.142754. Epub 2024 Jul 2.
Endocrine disrupting chemicals are of concern because of possible human health effects, thus they are frequently included in biomonitoring studies. Current analytical methods are focused on known chemicals and are incapable of identifying or quantifying other unknown chemicals and their metabolites. Non-targeted analysis (NTA) methods are advantageous since they allow for broad chemical screening, which provides a more comprehensive characterization of human chemical exposure, and can allow elucidation of metabolic pathways for unknown chemicals. There are still many challenges associated with NTA, which can impact the results obtained. The chemical space, i.e., the group of known and possible compounds within the scope of the method, must clearly be defined based on the sample preparation, as this is critical in identifying chemicals with confidence. Data acquisition modes and mobile phase additives used with liquid chromatography coupled to high-resolution mass-spectrometry can affect the chemicals ionized and structural identification based on the spectral quality. In this study, a sample preparation method was developed using a novel clean-up approach with CarbonS cartridges, for endocrine-disrupting chemicals in urine, including new bisphenol A analogues and benzophenone-based UV filters, like methyl bis (4-hydroxyphenyl acetate). The study showed that data dependent acquisition (DDA) had a lower identification rate (40%) at low spiking levels, i.e., 1 ng/mL, compared to data independent acquisition (DIA) (57%), when Compound Discoverer was used. In DDA, more compounds were identified using Compound Discoverer, with an identification rate of 95% when ammonium acetate was compared to acetic acid (82%) as a mobile phase additive. TraceFinder software had an identification rate of 53% at 1 ng/mL spiking level using the DDA data, compared to 40% using the DIA data. Using the developed method, 2,4 bisphenol F was identified for the first time in urine samples. The results show how NTA can provide human exposure information for risk assessment and regulatory action but standardized reporting of procedures is needed to ensure study results are reproducible and accurate. His Majesty the King in Right of Canada, as represented by the Minister of Health, 2024.
内分泌干扰化学物质引起关注是因为它们可能对人类健康产生影响，因此它们经常被纳入生物监测研究中。目前的分析方法侧重于已知的化学物质，无法识别或量化其他未知的化学物质及其代谢物。非靶向分析 (NTA) 方法具有优势，因为它们允许进行广泛的化学筛选，从而更全面地描述人类的化学暴露情况，并可以阐明未知化学物质的代谢途径。NTA 仍然存在许多挑战，这些挑战可能会影响结果。化学空间，即方法范围内已知和可能的化合物组，必须根据样品制备进行明确界定，因为这对于有信心地识别化学物质至关重要。与液相色谱-高分辨率质谱联用的采集模式和流动相添加剂会影响基于光谱质量电离和结构鉴定的化学物质。在这项研究中，开发了一种使用新型 CarbonS 小柱进行尿液中内分泌干扰化学物质净化的样品制备方法，包括新的双酚 A 类似物和基于二苯甲酮的紫外线滤光剂，如甲基双（4-羟基苯基）乙酸酯。研究表明，与数据独立采集 (DIA)（57%）相比，在使用 Compound Discoverer 时，数据依赖采集 (DDA) 在低添加水平（即 1ng/mL）下的鉴定率较低（40%）。在 DDA 中，使用 Compound Discoverer 鉴定出更多的化合物，当使用乙酸铵作为流动相添加剂时，鉴定率为 95%，而当使用乙酸时，鉴定率为 82%。使用 DDA 数据时，TraceFinder 软件的鉴定率为 53%，而使用 DIA 数据时为 40%。使用所开发的方法，首次在尿液样本中鉴定出 2,4-双酚 F。结果表明，NTA 如何为风险评估和监管行动提供人类暴露信息，但需要标准化报告程序以确保研究结果具有可重复性和准确性。加拿大卫生部长代表国王陛下，2024 年。
