Hynds Hannah M, Carpenter Jana M, Hines Kelly M
Department of Chemistry, University of Georgia, Athens, Georgia 30602, United States.
Anal Chem. 2025 Jul 8;97(26):13809-13816. doi: 10.1021/acs.analchem.5c00417. Epub 2025 Jun 24.
The implementation of mass spectrometry (MS) in clinical microbiology has made a significant improvement in the turnaround time from positive culture to identification, but current protein-based approaches can struggle with species-level identification because of the high degree of homology within a genus. However, other MS-based strategies for bacterial identification that are based on lipids and small molecules have shown promise toward species-level identification and detection of specific phenotypes, including those related to antibiotic resistance. We are leveraging rapid gas-phase ion mobility (IM) separations coupled to MS to simultaneously detect the lipids and metabolites in bacterial pathogens. Using flow-injection (FI) rather than liquid chromatography (LC), we instead rely more directly on the structural separation of the IM dimension to resolve features from different biochemical classes and aid in identification. A head-to-head comparison demonstrates that the FI-IM-MS multiomic strategy performs similarly to LC-IM-MS in its ability to distinguish 24 strains of the high-concern ESKAPE pathogens, while shortening overall analysis time from 17 to 2 min per injection. We demonstrate that the IM dimension has excellent stability and reproducibility, which enables extracted IM peak areas to be used in lieu of chromatographic peak areas. Furthermore, the same features that are important for the discrimination of bacterial species and strains are found within both the FI-IM-MS and HILIC-IM-MS data sets. These results showcase the capabilities of mobility-enabled rapid multiomics and open the possibility to detect subtle strain-level differences and resistance phenotypes in bacterial pathogens by including additional classes of biomolecules.
质谱(MS)技术在临床微生物学中的应用显著缩短了从阳性培养到鉴定的周转时间,但目前基于蛋白质的方法在种水平鉴定方面存在困难,因为同一属内的同源性程度很高。然而,其他基于质谱的细菌鉴定策略,即基于脂质和小分子的策略,在种水平鉴定和特定表型检测方面显示出了前景,包括与抗生素耐药性相关的表型。我们正在利用与质谱联用的快速气相离子迁移率(IM)分离技术,同时检测细菌病原体中的脂质和代谢物。使用流动注射(FI)而非液相色谱(LC),我们更直接地依赖于IM维度的结构分离来解析不同生化类别的特征并辅助鉴定。一项直接比较表明,FI-IM-MS多组学策略在区分24株高关注ESKAPE病原体的能力方面与LC-IM-MS表现相似,同时将每次进样的总体分析时间从17分钟缩短至2分钟。我们证明IM维度具有出色的稳定性和重现性,这使得提取的IM峰面积能够替代色谱峰面积使用。此外,在FI-IM-MS和亲水相互作用液相色谱-IM-MS(HILIC-IM-MS)数据集中都发现了对区分细菌种类和菌株很重要的相同特征。这些结果展示了基于迁移率的快速多组学的能力,并开启了通过纳入其他类别的生物分子来检测细菌病原体中细微菌株水平差异和耐药表型的可能性。