Bylund J, Ericsson J, Oliw E H
Department of Pharmaceutical Biosciences, Uppsala Biomedical Center, Uppsala University, Sweden.
Anal Biochem. 1998 Dec 1;265(1):55-68. doi: 10.1006/abio.1998.2897.
We have used reversed phase-high performance liquid chromatography-mass spectrometry (RP-HPLC-MS) with an ion trap mass spectrometer to study the metabolism of arachidonic and linoleic acids by human recombinant cytochrome P450 (CYP) enzymes. We first recorded the MS2 spectra of the carboxylate anions of epoxides, diols, omega-side chain, and bisallylic hydroxy fatty acids of arachidonic, octadeuterated arachidonic, and linoleic acids. The metabolites formed by CYP2C9 and CYP2C19 were then studied. CYP2C9 converted arachidonic and linoleic acids to epoxides/diols and monohydroxy fatty acids. Some hydroxyeicosatetraenoic acids (HETEs) were studied in detail to investigate the oxygenation mechanism. Incubation of CYP2C9 under oxygen-18 gas showed that all HETEs had incorporated oxygen-18 to the same degree. Chiral HPLC showed that CYP2C9 formed 15R-HETE (72% of the R enantiomer), 13S-HETE (90%), and 11R-HETE (57%). RP-HPLC-MS analysis revealed that CYP2C19 oxygenated arachidonic acid to 19-HETE, 14,15-epoxyeicosatrienoic acid (EET), and 8,9-EET as main metabolites. The method was sufficiently sensitive to identify arachidonic acid metabolites formed by some other isozymes. RP-HPLC-MS with MS2 seems to be useful for rapid identification of fatty acid metabolites in complex mixtures formed by cytochrome P450.
我们使用反相高效液相色谱 - 质谱联用仪(RP - HPLC - MS)和离子阱质谱仪来研究人重组细胞色素P450(CYP)酶对花生四烯酸和亚油酸的代谢。我们首先记录了花生四烯酸、十八氘代花生四烯酸和亚油酸的环氧化物、二醇、ω-侧链以及双烯丙基羟基脂肪酸的羧酸根阴离子的二级质谱(MS2)谱图。然后研究了CYP2C9和CYP2C19形成的代谢产物。CYP2C9将花生四烯酸和亚油酸转化为环氧化物/二醇和单羟基脂肪酸。对一些羟基二十碳四烯酸(HETEs)进行了详细研究以探究氧化机制。在18O2气体下孵育CYP2C9表明,所有HETEs掺入18O的程度相同。手性高效液相色谱显示CYP2C9形成15R - HETE(R对映体的72%)、13S - HETE(90%)和11R - HETE(57%)。RP - HPLC - MS分析表明,CYP2C19将花生四烯酸氧化为19 - HETE、14,15 - 环氧二十碳三烯酸(EET)和8,9 - EET作为主要代谢产物。该方法灵敏度足以鉴定由其他一些同工酶形成的花生四烯酸代谢产物。带有MS2的RP - HPLC - MS似乎有助于快速鉴定细胞色素P450在复杂混合物中形成的脂肪酸代谢产物。