人尿中BPA及其替代物的靶向定量和离子迁移率-HRMS可疑筛查
Target quantification and ion mobility-HRMS suspect screening of BPA and its alternatives in human urine.
摘要(中文译文)
双酚A（BPA）及其结构类似物因具有内分泌干扰特性且在人群中广泛暴露而成为备受关注的污染物。随着双酚A逐步被替代性双酚类物质取代，对能够监测生物基质中受监管及新兴类似物的灵敏分析方法的需求日益增加。本研究开发了一种基于超高效液相色谱-串联质谱（UHPLC-MS/MS）和离子迁移谱-高分辨质谱（IM-HRMS）的快速分析方法，用于人体尿液中双酚类物质的定量测定及可疑筛查鉴定。经酶解去结合和固相萃取后，采用UHPLC-MS/MS对双酚A及八种优先双酚类物质进行定量分析。方法验证结果显示良好的线性（r = 0.9976-0.9999）、定量限为0.1 ng/mL、相对回收率在89.1%至135.0%之间，中间精密度通常低于10.0%。将该方法应用于25名健康志愿者的尿液样本，发现双酚A、双酚S（BPS）和双酚F（BPF）的暴露普遍存在。为扩大化学覆盖范围，采用基于IM-HRMS的可疑筛查对相同提取物进行分析，鉴定出额外的双酚类物质，包括双酚G（BPG）和双酚M（BPM）。离子迁移谱的引入提供了碰撞截面积（CCS）值，并能够区分结构相关及同量异位化合物，提高了注释置信度。此外，本研究建立了双酚E（BPE）、BPG和BPM的新实验CCS参考值，扩展了目前可用的双酚类物质表征数据库。所提出的方法为监测人群对已知及新兴双酚类物质的暴露提供了综合策略，并支持未来的生物监测和风险评估研究。
Abstract
Bisphenol A (BPA) and its structural alternatives are contaminants of concern due to their endocrine-disrupting properties and widespread human exposure. The progressive replacement of BPA by alternative bisphenols has increased the need for sensitive analytical methods capable of monitoring both regulated and emerging analogues in biological matrices. In this study, a fast analytical approach based on ultra-high-performance liquid chromatography-tandem mass spectrometry (UHPLC-MS/MS) and ion mobility-high-resolution mass spectrometry (IM-HRMS) was developed for the determination and suspect screening identification of bisphenols in human urine. Following enzymatic deconjugation and solid-phase extraction, BPA and eight priority bisphenols were quantified by UHPLC-MS/MS. Method validation demonstrated excellent linearity (r = 0.9976-0.9999), limits of quantification of 0.1 ng/mL, relative recoveries between 89.1 and 135.0%, and intermediate precision generally below 10.0%. Application of the method to urine samples from 25 healthy volunteers revealed widespread exposure to BPA, bisphenol S (BPS), and bisphenol F (BPF). To extend chemical coverage, the same extracts were analyzed by IM-HRMS-based suspect screening, leading to the identification of additional bisphenols, including bisphenol G (BPG) and bisphenol M (BPM). The integration of IM provided collision cross section (CCS) values and enabled the discrimination of structurally related and isobaric compounds, improving annotation confidence. Furthermore, new experimental CCS reference values were established for bisphenol E (BPE), BPG, and BPM, expanding the currently available database for bisphenol characterization. The proposed approach provides a comprehensive strategy for monitoring human exposure to both of known and emerging bisphenols and supports future biomonitoring and risk assessment studies.
如何引用
AMA
Riccardo De Santo, Lucia Coppola, Fabiola Ferri, Cinzia La Rocca, Anna Laura Iamiceli. Target quantification and ion mobility-HRMS suspect screening of BPA and its alternatives in human urine.. Talanta. 2027; doi:10.1016/j.talanta.2026.130488.
APA
Riccardo De Santo, Lucia Coppola, Fabiola Ferri, Cinzia La Rocca, Anna Laura Iamiceli (2027). Target quantification and ion mobility-HRMS suspect screening of BPA and its alternatives in human urine.. Talanta. https://doi.org/10.1016/j.talanta.2026.130488
GB/T 7714
Riccardo De Santo, Lucia Coppola, Fabiola Ferri, Cinzia La Rocca, Anna Laura Iamiceli. Target quantification and ion mobility-HRMS suspect screening of BPA and its alternatives in human urine.[J]. Talanta, 2027 doi:10.1016/j.talanta.2026.130488.
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