Efficient Hydrogen–Deuterium Exchange in Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry Imaging for Confident Metabolite Identification
Efficient Hydrogen–Deuterium Exchange in Matrix-Assisted Laser Desorption/Ionization Mass Spectrometry Imaging for Confident Metabolite Identification
复制标题
基质辅助激光解吸/电离质谱成像中的高效氢-氘交换可实现可靠的代谢物鉴定
DOI：
10.1021/acs.analchem.2c00978
复制
发表时间：
2022
影响因子：
7.4
通讯作者：
Lee, Young Jin
中科院分区：
文献类型：
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作者：
Rensner, Josiah J.;Lee, Young Jin
高效的氢-氘交换（HDX）是一种用于低真空基质辅助激光解吸/电离（MALDI）质谱成像（MSI）的技术。通过将D2 O蒸气引入加热的MALDI源中并结合氘标记的基质，可以实现73-85%的HDX效率，这允许正确确定多达17个不稳定氢的可能H/D交换的数目。这提供了有价值的正交信息，以m/z，允许增加代谢物鉴定的信心，同时保留空间信息MSI供应。当与高通量METASPACE注释相结合时，这种方法可以系统地改善MALDI-MS成像中的非靶向代谢物注释。将该方法应用于浮萍顶面、底面和中段的MALDI-MS成像。在使用BraChem数据库使用10%的错误发现率进行的总共56个样本注释中，其中31个注释（55%）与我们的HDX数据匹配，提供了额外的置信度。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，大大提高了代谢物鉴定的信心。
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 supplementm/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 ofLemna minorfronds. 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.