Lang D H, Yeung C K, Peter R M, Ibarra C, Gasser R, Itagaki K, Philpot R M, Rettie A E
Department of Medicinal Chemistry, University of Washington, Seattle 98195, USA.
Biochem Pharmacol. 1998 Oct 15;56(8):1005-12. doi: 10.1016/s0006-2952(98)00218-4.
In the present study, we expressed human flavin-containing monooxygenase 1 (FMO1), FMO3, FMO4t (truncated), and FMO5 in the baculovirus expression vector system at levels of 0.6 to 2.4 nmol FMO/mg of membrane protein. These four isoforms, as well as purified rabbit FMO2, and eleven heterologously expressed human P450 isoforms were examined for their capacity to metabolize trimethylamine (TMA) to its N-oxide (TMAO), using a new, specific HPLC method with radiochemical detection. Human FMO3 was by far the most active isoform, exhibiting a turnover number of 30 nmol TMAO/nmol FMO3/min at pH 7.4 and 0.5 mM TMA. None of the other monooxygenases formed TMAO at rates greater than 1 nmol/nmol FMO/min under these conditions. Human fetal liver, adult liver, kidney and intestine microsomes were screened for TMA oxidation, and only human adult liver microsomes provided substantial TMAO-formation (range 2.9 to 9.1 nmol TMAO/mg protein/min, N = 5). Kinetic studies of TMAO formation by recombinant human FMO3, employing three different analytical methods, resulted in a Km of 28 +/- 1 microM and a Vmax of 36.3 +/- 5.7 nmol TMAO/nmol FMO3/min. The Km determined in human liver microsomes ranged from 13.0 to 54.8 microM. Therefore, at physiological pH, human FMO3 is a very specific and efficient TMA N-oxygenase, and is likely responsible for the metabolic clearance of TMA in vivo in humans. In addition, this specificity provides a good in vitro probe for the determination of FMO3-mediated activity in human tissues, by analyzing TMAO formation at pH 7.4 with TMA concentrations not higher than 0.5 mM.
在本研究中,我们在杆状病毒表达载体系统中表达了人含黄素单加氧酶1(FMO1)、FMO3、FMO4t(截短型)和FMO5,其表达水平为0.6至2.4 nmol FMO/毫克膜蛋白。使用一种新的、具有放射化学检测功能的特异性高效液相色谱法,检测了这四种同工型以及纯化的兔FMO2和十一种异源表达的人细胞色素P450同工型将三甲胺(TMA)代谢为其N-氧化物(TMAO)的能力。人FMO3是迄今为止活性最高的同工型,在pH 7.4和0.5 mM TMA条件下,其转换数为30 nmol TMAO/nmol FMO3/分钟。在这些条件下,其他单加氧酶形成TMAO的速率均不超过1 nmol/nmol FMO/分钟。对人胎儿肝脏、成人肝脏、肾脏和肠道微粒体进行了TMA氧化筛选,只有成人肝脏微粒体产生了大量的TMAO(范围为2.9至9.1 nmol TMAO/毫克蛋白/分钟,N = 5)。采用三种不同分析方法对重组人FMO3形成TMAO的动力学研究结果显示,Km为28±1 μM,Vmax为36.3±5.7 nmol TMAO/nmol FMO3/分钟。在人肝脏微粒体中测定的Km范围为13.0至54.8 μM。因此,在生理pH条件下,人FMO3是一种非常特异性且高效的TMA N-氧化酶,可能负责人体内TMA的代谢清除。此外,这种特异性为通过分析pH 7.4、TMA浓度不高于0.5 mM时TMAO的形成来测定人组织中FMO3介导的活性提供了一个良好的体外探针。