Ultra-High Mass Resolving Power, Mass Accuracy, and Dynamic Range MALDI Mass Spectrometry Imaging by 21-T FT-ICR MS
Ultra-High Mass Resolving Power, Mass Accuracy, and Dynamic Range MALDI Mass Spectrometry Imaging by 21-T FT-ICR MS
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DOI：
10.1021/acs.analchem.9b04768
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发表时间：
2020-02-18
影响因子：
7.4
通讯作者：
Smith, Donald F.
中科院分区：
文献类型：
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作者：
Bowman, Andrew P.;Blakney, Greg T.;Smith, Donald F.
通过基质辅助激光解吸/电离 (MALDI) 质谱成像 (MSI) 对复杂生物表面进行详细表征需要具有高质量分辨率、质量精度和动态范围的仪器。傅里叶变换离子回旋共振质谱 (FT-ICR MS) 为 MALDI MSI 实验提供最高的质谱性能，并且经常揭示低性能仪器无法解析的分子特征。更高的磁场强度改善了 FT-ICR 的所有性能特征；质量分辨能力线性提高，而质量精度和动态范围随磁场强度呈二次方提高。在这里，首次展示了 21T 的 MALDI MSI：通过对生物组织切片的直接分析获得了超过 1 600 000（m/z 400）的质量分辨率、低于 100 ppb 的均方根质量测量精度以及超过 500:1 的每像素动态范围。 m/z 差异小至 1.79 mDa 的分子特征得到解析并以高质量精度进行鉴定。这些特征允许分离和识别组织底层结构的脂质。 21T MALDI FT-ICR MSI 实验结合了独特的分子细节、准确性、灵敏度和动态范围，使研究人员能够可视化迄今为止一直隐藏的复杂组织中的分子结构。所述仪器允许未来的创新，例如高端研究，以无与伦比的细节揭示生物、地质和工程有机材料表面的复杂性。
Detailed characterization of complex biological surfaces by matrix-assisted laser desorption/ionization (MALDI) mass spectrometry imaging (MSI) requires instrumentation that is capable of high mass resolving power, mass accuracy, and dynamic range. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) offers the highest mass spectral performance for MALDI MSI experiments, and often reveals molecular features that are unresolved on lower performance instrumentation. Higher magnetic field strength improves all performance characteristics of FT-ICR; mass resolving power improves linearly, while mass accuracy and dynamic range improve quadratically with magnetic field strength. Here, MALDI MSI at 21T is demonstrated for the first time: mass resolving power in excess of 1 600 000 (at m/z 400), root-mean-square mass measurement accuracy below 100 ppb, and dynamic range per pixel over 500:1 were obtained from the direct analysis of biological tissue sections. Molecular features with m/z differences as small as 1.79 mDa were resolved and identified with high mass accuracy. These features allow for the separation and identification of lipids to the underlying structures of tissues. The unique molecular detail, accuracy, sensitivity, and dynamic range combined in a 21T MALDI FT-ICR MSI experiment enable researchers to visualize molecular structures in complex tissues that have remained hidden until now. The instrument described allows for future innovative, such as high-end studies to unravel the complexity of biological, geological, and engineered organic material surfaces with an unsurpassed detail.