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二硫化钼表面改性纳米材料作为表面辅助激光解吸附/离子化质谱基质用于血浆中弱极性脂类的检测
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摘要
传统的基质辅助激光解吸附/离子化技术(matrix-assisted laser desorption/ionization,MALDI),采用有机小分子酸作为基质,会在低分子质量区形成背景干扰,阻碍了该技术在小分子分析方面的应用;基质形成不均匀结晶,又会阻碍该技术在定量方面的应用。表面辅助激光解吸附/离子化技术(surface-assisted laser desorption/ionization,SALDI)采用无机材料作为基质,无机材料不结晶,不挥发,不会造成背景污染,可用于小分子的分析。该技术还具有重现性好、耐盐度高、上样方法灵活等优点。文献中报道了各种碳材料、硅材料、金属及金属氧化物材料作为基质,用于小分子的分析。本课题组新开发了表面改性的二硫化钼纳米材料MoS_2@3-MPA,MoS_2@MBA,MoS_2@Cys作为SALDI基质,用于血浆中弱极性脂类的检测。首先对表面改性试剂进行了优化,结果表明MoS_2@3-MPA基质材料具有最好的效果;之后对脂类萃取方法进行了优化,结果表明正丁醇萃取法有最好的萃取效果。该检测方法上样灵活,重现性好。采用MoS_2@3-MPA作为基质,可以检测到血浆中的甘油三酯、甘油二酯、乳糖基/半乳糖基神经酰胺等弱极性脂类。脂类主要以钠离子加合物[M+Na]~+的形式被检测到。方法可用作血浆中弱极性脂类的分析。
The use of organic matrix hindered the application of matrix assisted laser desorption/ionization mass spectrometry,MALDI-MS,for the analysis of small molecules.The problem could be solved by using inorganic materials as matrix,which termed surface assisted laser desorption/ionization mass spectrometry,SALDI-MS.The latter one proved to have better reproducibility,higher salt tolerance and flexible sampling approaches.Various materials including carbon-,silicon-,metal-and metal oxide-materials have been tested as SALDI matrices.In this work,surface modified MoS_2 nano-materials were applied as SALDI matrix for the detection of lipids in plasma.Surface modification agents and lipid extraction methods were optimized to get the optical results.MoS2@3-MPA proved to be the best matrix.Lipids were observed as sodium adducts,and most of the lipids were TAG and DAG.The method showed good potential for the analysis of apolar lipids in plasma.
引文
[1]Wang,T.Y.;Gao,D.L.;Zhou,J.Q.;Zhu,Z.W.;Papakonstantinou,P.;Yan,L;Li,M.X.Chem.Eur.J.2013,19:11939.
    [2]Alshehry,Z.H.;Barlow,C.K.;Weir,J.M.;Zhou,Y.P.;Mcconville,M.J.;Meikle,P.J.Metabolites 2015,5:389.

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