Spatiochemically Profiling Microbial Interactions with Membrane Scaffolded Desorption Electrospray Ionization-Ion Mobility-Imaging Mass Spectrometry and Unsupervised Segmentation
Spatiochemically Profiling Microbial Interactions with Membrane Scaffolded Desorption Electrospray Ionization-Ion Mobility-Imaging Mass Spectrometry and Unsupervised Segmentation
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DOI：
10.1021/acs.analchem.9b02992
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发表时间：
2019-11-05
影响因子：
7.4
通讯作者：
McLean, John A.
中科院分区：
文献类型：
--
作者：
Ellis, Berkley M.;Fischer, Caleb N.;McLean, John A.
对微生物小分子相互作用的清单进行成像为微生物化学生态学和人类医学提供了重要的见解。在这里，我们展示了一种新的方法，用于增强检测和分析存在于微生物表面的种间相互作用的代谢物。我们表明，解吸电喷雾电离成像质谱（ESIMS）使用微孔膜支架（MMS），使测试样品制备技术之间的相互作用的微生物的增强空间化学分析。与基质辅助激光解吸电离（MALDI）和其他IMS方法相比，通过直接IMS原位分析微生物化学，膜支架的IMS-IMS具有固有的优势。当与通过MMS ESI-IMS非介导采样的液相色谱电喷雾电离-质谱（LC-ESI-MS）相比时，这种快速成像方法产生灵敏的MS分析，具有独特的m/z测量值。无监督分割成像分析所获得的EST-IMS数据揭示了不同的化学区域对应于微生物间的现象，如捕食和通信。我们通过将粘病毒素A和DKxanthene-560分别与其已知的捕食和相位变化的生物学作用相关联来验证该方法。除了提供已知的天然产品的第一个地形位置，我们优先考虑54个未知的功能，使用分割的捕食区域内。因此，EST-IMS和无监督分割在空间上注释了粘细菌的已知生物学，并提供了新的未表征的小分子的功能探索。
Imaging the inventory of microbial small molecule interactions provides important insights into microbial chemical ecology and human medicine. Herein we demonstrate a new method for enhanced detection and analysis of metabolites present in interspecies interactions of microorganisms on surfaces. We demonstrate that desorption electrospray ionization-imaging mass spectrometry (DESI-IMS) using microporous membrane scaffolds (MMS) enables enhanced spatiochemical analyses of interacting microbes among tested sample preparation techniques. Membrane scaffolded DESI-IMS has inherent advantages compared to matrix-assisted laser desorption ionization (MALDI) and other IMS methods through direct IMS analyses of microbial chemistry in situ. This rapid imaging method yields sensitive MS analyses with unique m/z measurements when compared to liquid chromatography electrospray ionization-mass spectrometry (LC-ESI-MS) via unmediated sampling by MMS DESI-IMS. Unsupervised segmentation imaging analysis of acquired DESI-IMS data reveals distinct chemical regions corresponding to intermicrobial phenomenon such as predation and communication. We validate the method by linking Myxovirescin A and DKxanthene-560 to their known biological roles of predation and phase variation, respectively. In addition to providing the first topographic locations of known natural products, we prioritize 54 unknown features using segmentation within the region of predation. Thus, DESI-IMS and unsupervised segmentation spatially annotates the known biology of myxobacteria and provides functional exploration of newly uncharacterized small molecules.