Izquierdo-Sandoval David, Sancho Juan Vicente, Hernández Félix, Portoles Tania
Environmental and Public Health Analytical Chemistry, Research Institute for Pesticides and Water (IUPA), Universitat Jaume I, Av. Sos Baynat S/N, Castellón de la Plana 12071, Spain.
Environ Sci Technol. 2025 Feb 11;59(5):2436-2448. doi: 10.1021/acs.est.4c11032. Epub 2025 Jan 31.
This study explores the capabilities of GC-APCI-IMS-QTOF MS and GC-EI-QOrbitrap MS in screening applications and different strategies for wide-scope screening of organic microcontaminants using target suspect and nontarget approaches. On one side, GC-APCI-IMS-QTOF MS excels at preserving molecular information and adds ion mobility separation, facilitating screening through the list of componentized features containing accurate mass, retention time, CCS, and fragmentation data. On the other side, the extensive and robust fragmentation of GC-EI-QOrbitrap MS allows the application of different strategies for target and nontarget approaches using the NIST library spectra. Our findings revealed that GC-EI-QOrbitrap MS is more sensitive in target approaches. Automated workflows for suspect screening in GC-APCI-IMS-QTOF MS minimize false annotations but face challenges with false negatives due to in-source fragmentation and limitations when using fragmentation tools. Conversely, a nontarget approach in GC-EI-QOrbitrap MS can reliably identify unknowns but results in more false annotations in complex matrices. This work highlights the strengths and limitations of each system and guides for their optimal application for wide-scope screening in environmental and food safety applications.
本研究探讨了气相色谱-大气压化学电离-离子迁移谱-四极杆飞行时间质谱（GC-APCI-IMS-QTOF MS）和气相色谱-电子轰击电离-四极杆轨道阱质谱（GC-EI-QOrbitrap MS）在筛选应用中的能力，以及使用目标物、可疑物和非目标物方法对有机微污染物进行宽范围筛选的不同策略。一方面，GC-APCI-IMS-QTOF MS在保留分子信息方面表现出色，并增加了离子迁移率分离，便于通过包含精确质量、保留时间、碰撞截面（CCS）和碎片数据的成分特征列表进行筛选。另一方面，GC-EI-QOrbitrap MS广泛而强大的碎片裂解功能允许使用美国国家标准与技术研究院（NIST）库谱图对目标物和非目标物方法应用不同的策略。我们的研究结果表明，GC-EI-QOrbitrap MS在目标物方法中更灵敏。GC-APCI-IMS-QTOF MS中用于可疑物筛选的自动化工作流程可最大限度地减少错误注释，但由于源内裂解以及使用裂解工具时的局限性，面临假阴性的挑战。相反，GC-EI-QOrbitrap MS中的非目标物方法可以可靠地识别未知物，但在复杂基质中会导致更多错误注释。这项工作突出了每个系统的优势和局限性，并为它们在环境和食品安全应用中的宽范围筛选的最佳应用提供了指导。
