Fatty acidomics: global analysis of lipid species containing a carboxyl group with a charge-remote fragmentation-assisted approach.
Fatty acidomics: global analysis of lipid species containing a carboxyl group with a charge-remote fragmentation-assisted approach.
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DOI：
10.1021/ac402078p
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发表时间：
2013-10-01
影响因子：
7.4
通讯作者：
Han, Xianlin
中科院分区：
文献类型：
--
作者：
Wang, Miao;Han, Rowland H.;Han, Xianlin
电荷远程裂解已被广泛认为是长脂肪链解离的一种有效方法。在此，我们利用这种方法，通过酰胺化反应对一种带电荷试剂进行一步衍生化后，利用电喷雾电离串联质谱（ESI - MS/MS）对所有脂肪酸（包括饱和、不饱和及修饰的脂肪酸）进行结构鉴定。我们针对疏水性、电荷强度以及电荷到羧基的距离，用不同的带电荷试剂对该方法进行了测试。我们发现，无论试剂的化学和物理性质如何不同，用这些试剂得到的所有衍生物都能产生有信息价值的电荷远程裂解模式，并且这些有信息价值的裂解模式都可有效地用于含羧基脂质种类的结构解析。我们还发现，脂肪酸异构体独特的电荷远程裂解使我们无需任何色谱分离就能确定这些异构体的组成。最后，单个衍生部分产生的丰富碎片使我们能够灵敏地对含羧基的单个种类进行定量。所描述的方法是对基于多维质谱的鸟枪法脂质组学的极大扩展，可用于对包括异构体和修饰物在内的脂肪酸进行全面分析。我们相信，这种方法能够极大地促进对众多病理状况背后的生化机制的鉴定。
Charge-remote fragmentation has been well recognized as an effective approach for dissociation of long aliphatic chains. Herein, we exploited this approach for structural identification of all fatty acids including saturated, unsaturated, and modified ones by using electrospray ionization tandem mass spectrometry (ESI-MS/MS) after one-step derivatization of a charge-carried reagent through an amidation reaction. We tested the approach with different charge-carried reagents with respective to the hydrophobicity, charge strength, and distance from the charge to the carboxyl group. We found all the derivatives with these reagents could yield informative charge-remote fragmentation patterns regardless of the different chemical and physical properties of the reagents and these informative fragmentation patterns all could be effectively used for structural elucidation of lipid species containing a carboxyl group. We further found that the distinguished charge-remote fragmentations of fatty acid isomers enabled us to determine the composition of these isomers without any chromatographic separation. Finally, the abundant fragments yielded from individual derivatized moiety enabled us to sensitively quantify the individual species containing a carboxyl group. The described approach was a great extension to the multidimensional mass spectrometry-based shotgun lipidomics for global analysis of fatty acids including isomers and modifications. We believe that this approach could greatly facilitate the identification of the biochemical mechanisms underlying numerous pathological conditions.
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DOI：
10.1016/s0021-9673(01)95986-2
发表时间：
1991-03-22
期刊：
JOURNAL OF CHROMATOGRAPHY
影响因子：
--
作者：
FAY, L;RICHLI, U
通讯作者：
RICHLI, U
影响因子：
2.9
作者：
Kotani, A;Fuse, T;Kusu, F
通讯作者：
Kusu, F
早期阿尔茨海默病的代谢组学：使用鸟枪脂质组学鉴定改变的血浆鞘脂组。
影响因子：
3.7
作者：
Han X;Rozen S;Boyle SH;Hellegers C;Cheng H;Burke JR;Welsh-Bohmer KA;Doraiswamy PM;Kaddurah-Daouk R
通讯作者：
Kaddurah-Daouk R
影响因子：
6.5
作者：
Han, Rowland H.;Wang, Miao;Han, Xianlin
通讯作者：
Han, Xianlin
影响因子：
3.1
作者：
Mochizuki, Yuko;Inagaki, Shinsuke;Toyo'oka, Toshimasa
通讯作者：
Toyo'oka, Toshimasa