In-Silico-Generated Library for Sensitive Detection of 2-Dimethylaminoethylamine Derivatized FAHFA Lipids Using High-Resolution Tandem Mass Spectrometry.,Analytical Chemistry

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In-Silico-Generated Library for Sensitive Detection of 2-Dimethylaminoethylamine Derivatized FAHFA Lipids Using High-Resolution Tandem Mass Spectrometry.
Analytical Chemistry ( IF 6.7 ) Pub Date : 2020-03-31 , DOI: 10.1021/acs.analchem.0c00172
Jun Ding _{1,

2} , Tobias Kind ₁ , Quan-Fei Zhu ₂ , Yu Wang ₂ , Jing-Wen Yan ₂ , Oliver Fiehn ₁ , Yu-Qi Feng _{2,

3}

Affiliation

Fatty acid esters of hydroxy fatty acids (FAHFAs) are a family of recently discovered lipids with important physiological functions in mammals and plants. However, low detection sensitivity in negative ionization mode mass spectrometry makes low-abundance FAHFA challenging to analyze. A 2-dimethylaminoethylamine (DMED) based chemical derivatization strategy was recently reported to improve the MS sensitivity of FAHFAs by labeling FAHFAs with a positively ionizable tertiary amine group. To facilitate reliable, high-throughput, and automatic annotation of these compounds, a DMED-FAHFA in silico library containing 4290 high-resolution tandem mass spectra covering 264 different FAHFA classes was developed. The construction of the library was based on the heuristic information from MS/MS fragmentation patterns of DMED-FAHFA authentic standards, and then, the patterns were applied to computer-generated DMED-FAHFAs. The developed DMED-FAHFA in silico library was demonstrated to be compatible with library search software NIST MS Search and the LC-MS/MS data processing tool MS-DIAL to guarantee high-throughput and automatic annotations. Applying the in silico library in Arabidopsis thaliana samples for profiling FAHFAs by high-resolution LC-MS/MS enabled the annotation of 19 DMED-FAHFAs from 16 families, including 3 novel compounds. Using the in silico library largely decreased the false-positive annotation rate in comparison to low-resolution LC-MS/MS. The developed library, MS/MS spectra, and development templates are freely available for commercial and noncommercial use at https://zenodo.org/record/3606905.

中文翻译：

使用高分辨率串联质谱法灵敏检测 2-二甲氨基乙胺衍生的 FAHFA 脂质的计算机生成库。

羟基脂肪酸的脂肪酸酯（FAHFA）是最近发现的一类脂质，在哺乳动物和植物中具有重要的生理功能。然而，负电离模式质谱检测灵敏度低，使得低丰度 FAHFA 的分析具有挑战性。最近报道了一种基于 2-二甲氨基乙胺 (DMED) 的化学衍生化策略，通过用可正电离的叔胺基团标记 FAHFA 来提高 FAHFAs 的 MS 灵敏度。为了促进这些化合物的可靠、高通量和自动注释，我们开发了一个 DMED-FAHFA 计算机库，其中包含 4290 个高分辨率串联质谱，涵盖 264 个不同的 FAHFA 类别。文库的构建基于 DMED-FAHFA 真实标准品的 MS/MS 碎片模式的启发式信息，然后将这些模式应用于计算机生成的 DMED-FAHFA。所开发的 DMED-FAHFA in silico 文库经证明与文库检索软件 NIST MS Search 和 LC-MS/MS 数据处理工具 MS-DIAL 兼容，以保证高通量和自动注释。应用拟南芥样品中的计算机文库通过高分辨率 LC-MS/MS 分析 FAHFA，能够注释来自 16 个家族的 19 种 DMED-FAHFA，其中包括 3 种新化合物。与低分辨率 LC-MS/MS 相比，使用计算机文库大大降低了假阳性注释率。开发的库、MS/MS 谱图和开发模板可免费用于商业和非商业用途，网址为 https://zenodo.org/record/3606905。

更新日期：2020-04-23

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