Departments of Pharmacology and Toxicology, Paul and Carole Stark Neurosciences Research Institute, Indiana University School of Medicine, Indianapolis, IN 46202, USA.
ACS Chem Neurosci. 2013 Mar 20;4(3):463-74. doi: 10.1021/cn300188h. Epub 2013 Jan 16.
Lacosamide ((R)-1) is a recently marketed, first-in-class, antiepileptic drug. Patch-clamp electrophysiology studies are consistent with the notion that (R)-1 modulates voltage-gated Na(+) channel function by increasing and stabilizing the slow inactivation state without affecting fast inactivation. The molecular pathway(s) that regulate slow inactivation are poorly understood. Affinity baits are chemical reactive units, which when appended to a ligand (drug) can lead to irreversible, covalent modification of the receptor thus permitting drug binding site identification including, possibly, the site of ligand function. We describe, herein, the synthesis of four (R)-1 affinity baits, (R)-N-(4″-isothiocyanatobiphenyl-4'-yl)methyl 2-acetamido-3-methoxypropionamide ((R)-8), (S)-N-(4″-isothiocyanatobiphenyl-4'-yl)methyl 2-acetamido-3-methoxypropionamide ((S)-8), (R)-N-(3″-isothiocyanatobiphenyl-4'-yl)methyl 2-acetamido-3-methoxypropionamide ((R)-9), and (R)-N-(3″-acrylamidobiphenyl-4'-yl)methyl 2-acetamido-3-methoxypropionamide ((R)-10). The affinity bait compounds were designed to interact with the receptor(s) responsible for (R)-1-mediated slow inactivation. We show that (R)-8 and (R)-9 are potent inhibitors of Na(+) channel function and function by a pathway similar to that observed for (R)-1. We further demonstrate that (R)-8 function is stereospecific. The calculated IC50 values determined for Na(+) channel slow inactivation for (R)-1, (R)-8, and (R)-9 were 85.1, 0.1, and 0.2 μM, respectively. Incubating (R)-9 with the neuronal-like CAD cells led to appreciable levels of Na(+) channel slow inactivation after cellular wash, and the level of slow inactivation only modestly decreased with further incubation and washing. Collectively, these findings have identified a promising structural template to investigate the voltage-gated Na(+) channel slow inactivation process.
拉科酰胺((R)-1)是一种最近上市的、具有首创性的抗癫痫药物。膜片钳电生理学研究表明,(R)-1 通过增加和稳定慢失活状态来调节电压门控 Na(+)通道功能,而不影响快速失活。调节慢失活的分子途径知之甚少。亲和诱饵是化学反应单元,当附加到配体(药物)上时,会导致受体不可逆的、共价修饰,从而允许鉴定药物结合位点,包括可能的配体功能位点。本文描述了四种(R)-1 亲和诱饵的合成,(R)-N-(4″-异硫氰酸基联苯-4′-基)甲基 2-乙酰氨基-3-甲氧基丙酰胺((R)-8)、(S)-N-(4″-异硫氰酸基联苯-4′-基)甲基 2-乙酰氨基-3-甲氧基丙酰胺((S)-8)、(R)-N-(3″-异硫氰酸基联苯-4′-基)甲基 2-乙酰氨基-3-甲氧基丙酰胺((R)-9)和(R)-N-(3″-丙烯酰胺基联苯-4′-基)甲基 2-乙酰氨基-3-甲氧基丙酰胺((R)-10)。亲和诱饵化合物旨在与负责(R)-1 介导慢失活的受体相互作用。结果表明,(R)-8 和 (R)-9 是钠离子通道功能的有效抑制剂,其作用途径与观察到的 (R)-1 相似。进一步证明(R)-8 的功能是立体特异性的。Na(+)通道慢失活的计算 IC50 值分别为(R)-1、(R)-8 和 (R)-9 为 85.1、0.1 和 0.2 μM。将 (R)-9 与神经元样 CAD 细胞孵育后,细胞洗涤后会导致钠离子通道明显的慢失活,进一步孵育和洗涤后,慢失活程度仅略有下降。总的来说,这些发现确定了一个有前途的结构模板,用于研究电压门控 Na(+)通道慢失活过程。