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High-resolution imaging and identification of biomolecules using Nano-DESI coupled to ion mobility spectrometry
Analytica Chimica Acta ( IF 6.2 ) Pub Date : 2021-09-21 , DOI: 10.1016/j.aca.2021.339085
Daisy Unsihuay 1 , Ruichuan Yin 1 , Daniela Mesa Sanchez 1 , Manxi Yang 1 , Yingju Li 2 , Xiaofei Sun 2 , Sudhansu K Dey 2 , Julia Laskin 1
Affiliation  

Simultaneous spatial localization and structural characterization of molecules in complex biological samples currently represents an analytical challenge for mass spectrometry imaging (MSI) techniques. In this study, we describe a novel experimental platform, which substantially expands the capabilities and enhances the depth of chemical information obtained in high spatial resolution MSI experiments performed using nanospray desorption electrospray ionization (nano-DESI). Specifically, we designed and constructed a portable nano-DESI MSI platform and coupled it with a drift tube ion mobility (IM) spectrometer-mass spectrometer. We demonstrate imaging of drift time-separated ions with a high spatial resolution of better than ∼25 μm using uterine tissues on day 4 of pregnancy in mice. Collision cross-section measurements provide unique molecular descriptors of molecules observed in nano-DESI-IM-MSI necessary for their unambiguous identification by comparison with databases. Meanwhile, isomer-specific imaging reveals variations in the isomeric composition across the tissue. Furthermore, IM separation efficiently eliminates isobaric and isomeric interferences originating from solvent peaks, overlapping isotopic peaks of endogenous molecules extracted from the tissue, and products of in-source fragmentation, which is critical to obtaining accurate concentration gradients in the sample using MSI. The structural information provided by the IM separation substantially expands the molecular specificity of high-resolution MSI necessary for unraveling the complexity of biological systems.



中文翻译:

使用 Nano-DESI 耦合离子迁移谱法进行生物分子的高分辨率成像和鉴定

目前,复杂生物样品中分子的同时空间定位和结构表征是质谱成像 (MSI) 技术的分析挑战。在这项研究中,我们描述了一个新的实验平台,它大大扩展了能力并增强了在使用纳喷雾解吸电喷雾电离 (nano-DESI) 进行的高空间分辨率 MSI 实验中获得的化学信息的深度。具体来说,我们设计并构建了一个便携式 nano-DESI MSI 平台,并将其与漂移管离子淌度 (IM) 质谱仪耦合。我们展示了在小鼠怀孕第 4 天使用子宫组织对漂移时间分离离子进行的成像,其空间分辨率优于~25 μm。碰撞截面测量提供了在 nano-DESI-IM-MSI 中观察到的分子的独特分子描述符,这是通过与数据库进行比较来明确识别它们所必需的。同时,异构体特异性成像揭示了整个组织中异构体组成的变化。此外,IM 分离有效地消除了源自溶剂峰、从组织中提取的内源性分子的重叠同位素峰以及源内碎裂产物的同位素和同分异构体干扰,这对于使用 MSI 获得样品中的准确浓度梯度至关重要。IM 分离提供的结构信息大大扩展了揭示生物系统复杂性所必需的高分辨率 MSI 的分子特异性。

更新日期:2021-10-01
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