Efficient Hydrogen–Deuterium Exchange in Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry Imaging for Confident Metabolite Identification,Analytical Chemistry

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Efficient Hydrogen–Deuterium Exchange in Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry Imaging for Confident Metabolite Identification
Analytical Chemistry ( IF 6.7 ) Pub Date : 2022-08-02 , DOI: 10.1021/acs.analchem.2c00978
Josiah J Rensner ₁ , Young Jin Lee ₁

Affiliation

Highly efficient hydrogen–deuterium exchange (HDX) is developed for mass spectrometry imaging (MSI) with low-vacuum matrix-assisted laser desorption/ionization (MALDI). A HDX efficiency of 73–85% is achieved by introducing D₂O vapor into a heated MALDI source in combination with a deuterium-labeled matrix, which allows correct determination of the number of possible H/D exchanges for up to 17 labile hydrogens. This provides valuable orthogonal information to supplement m/z, allowing for increased confidence in metabolite identification while retaining the spatial information MSI supplies. When combined with high-throughput METASPACE annotation, this approach can systematically improve untargeted metabolite annotations in MALDI-MS imaging. The developed method was applied to MALDI-MS imaging of the top surface, bottom surface, and middle section of Lemna minor fronds. Out of a total of 56 on-sample annotations made with the BraChem database using a 10% false discovery rate, 31 of these annotations (55%) matched our HDX data, providing additional confidence. For the remaining 45%, our data allowed us to narrow down structural possibilities and eliminate incorrect structures, greatly increasing confidence in metabolite identification.

中文翻译：

基质辅助激光解吸/电离质谱成像中的高效氢-氘交换用于可靠的代谢物鉴定

高效氢氘交换 (HDX) 被开发用于具有低真空基质辅助激光解吸/电离 (MALDI) 的质谱成像 (MSI)。_{通过将 D 2} O 蒸汽引入加热的 MALDI 源并结合氘标记的基质，可以实现 73–85% 的 HDX 效率，这可以正确确定多达 17 个不稳定氢的可能 H/D 交换的数量。这提供了有价值的正交信息来补充m / z，允许在保留 MSI 提供的空间信息的同时增加对代谢物鉴定的信心。当与高通量 METASPACE 注释相结合时，这种方法可以系统地改进 MALDI-MS 成像中的非靶向代谢物注释。将所开发的方法应用于Lemna小叶的顶面、底面和中间部分的 MALDI-MS 成像。在使用 BraChem 数据库以 10% 的错误发现率进行的总共 56 个样本注释中，其中 31 个 (55%) 与我们的 HDX 数据匹配，提供了额外的信心。对于剩下的 45%，我们的数据使我们能够缩小结构可能性并消除不正确的结构，从而大大提高了对代谢物鉴定的信心。

更新日期：2022-08-02

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