High-Definition Differential Ion Mobility Spectrometry with Structural Isotopic Shifts for Anionic Compounds
High-Definition Differential Ion Mobility Spectrometry with Structural Isotopic Shifts for Anionic Compounds
复制标题
具有阴离子化合物结构同位素位移的高清晰度差分离子淌度光谱法
DOI：
10.1021/jasms.3c00190
复制
发表时间：
2023
影响因子：
3.2
通讯作者：
Shvartsburg, Alexandre A.
中科院分区：
文献类型：
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作者：
Pathak, Pratima;Shvartsburg, Alexandre A.
微分离子迁移谱 (FAIMS) 于 2000 年代出现，是与质谱 (MS) 结合使用的一种新型定位分离工具。十年前推出的高清 FAIMS 已经能够解析具有微小结构变化的肽、脂质和其他分子异构体，最近还可以进行同位素位移分析，其中稳定同位素的光谱模式可对离子几何形状进行指纹识别。这些研究，包括所有同位素位移分析，均处于积极模式。在这里，我们对以邻苯二甲酸异构体为例的阴离子实现了相同的高分辨率。同位素位移的分辨能力和幅度与类似卤代苯胺阳离子的指标一致，建立具有结构特定同位素位移的高清负模式 FAIMS。不同的位移（包括新的 18O）保持相加且相互正交，证明了这些特性在元素和电荷状态上的普遍性。扩展到常见（非卤化）有机化合物是 FAIMS 同位素变换方法广泛使用的关键一步。
Differential ion mobility spectrometry (FAIMS) had emerged in the 2000s as a novel tool for postionization separations in conjunction with mass spectrometry (MS). High-definition FAIMS introduced a decade ago has enabled resolution of peptide, lipid, and other molecular isomers with minute structural variations and recently the isotopic shift analyses where the spectral pattern for stable isotopes fingerprints the ion geometry. Those studies, including all isotopic shift analyses, were in the positive mode. Here, we achieve the same high resolution for anions exemplified by phthalic acid isomers. The resolving power and magnitude of isotopic shifts are in line with the metrics for analogous haloaniline cations, establishing high-definition negative-mode FAIMS with structurally specific isotopic shifts. Different shifts (including the new18O) remain additive and mutually orthogonal, demonstrating the generality of those properties across the elements and charge states. Expanding to common (not halogenated) organic compounds is a key step toward the broad use of FAIMS isotopic shift methodology.