Immuno‐Desorption Electrospray Ionization Mass Spectrometry Imaging Identifies Functional Macromolecules by Using Microdroplet‐Cleavable Mass Tags
Immuno‐Desorption Electrospray Ionization Mass Spectrometry Imaging Identifies Functional Macromolecules by Using Microdroplet‐Cleavable Mass Tags
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免疫解吸电喷雾电离质谱成像通过使用微滴可切割质量标签识别功能性大分子
DOI：
10.1002/anie.202216969
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通讯作者：
Richard Neil Zare
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作者：
Xiaowei Song;Qingce Zang;Chao Li;Tianhao Zhou;Richard Neil Zare
我们提出了基于免疫分析的解吸电喷雾电离质谱成像（immuno-DESI-MSI）来可视化功能性大分子，例如药物靶点和级联信号因子。合成了一组硼酸质量标签 (BMT) 以标记抗体作为 MSI 探针。硼酸酯键用于交联 BMT 与半乳糖胺修饰的抗体。 BMT 可以通过硼酸酯键的超快裂解而从其束缚的抗体中释放出来，这种裂解是由喷射的含有水的 DESI 微滴的酸性条件引起的。荧光部分使 BMT 能够在光学和 MS 成像模式下工作。带正电荷的季铵基团提高了电离效率。由于其独特的同位素模式，硼元素的引入也使得质量标签易于识别。免疫-DESI-MSI 提供了一种有吸引力的策略，可以对大分子进行空间图谱分析，超出了传统 DESI-MSI 所能观察到的范围，只要抗体可用于感兴趣的目标分子。
We present immunoassay‐based desorption electrospray ionization mass spectrometry imaging (immuno‐DESI‐MSI) to visualize functional macromolecules such as drug targets and cascade signaling factors. A set of boronic acid mass tags (BMTs) were synthesized to label antibodies as MSI probes. The boronic ester bond is employed to cross‐link the BMT with the galactosamine‐modified antibody. The BMT can be released from its tethered antibody by ultrafast cleavage of the boronic ester bond caused by the acidic condition of sprayed DESI microdroplets containing water. The fluorescent moiety enables the BMT to work in both optical and MS imaging modes. The positively charged quaternary ammonium group enhances the ionization efficiency. The introduction of the boron element also makes mass tags readily identified because of its unique isotope pattern. Immuno‐DESI‐MSI provides an appealing strategy to spatially map macromolecules beyond what can be observed by conventional DESI‐MSI, provided antibodies are available to the targeted molecules of interest.