Hamel P, Riendeau D, Brideau C, Chan C C, Desmarais S, Delorme D, Dubé D, Ducharme Y, Ethier D, Grimm E, Falgueyret J P, Guay J, Jones T R, Kwong E, McAuliffe M, McFarlane C S, Piechuta H, Roumi M, Tagari P, Young R N, Girard Y
Merck Frosst Centre for Therapeutic Research, Pointe Claire-Dorval, Quebec, Canada.
J Med Chem. 1997 Aug 29;40(18):2866-75. doi: 10.1021/jm970046b.
Dioxabicyclooctanyl naphthalenenitriles have been reported as a class of potent and nonredox 5-lipoxygenase (5-LO) inhibitors. These bicyclo derivatives were shown to be metabolically more stable than their tetrahydropyranyl counterparts but were not well orally absorbed. Replacement of the phenyl ring in the naphthalenenitrile 1 by a pyridine ring leads to the potent and orally absorbed inhibitor 3g (L-739,010, 2-cyano-4-(3-furyl)-7-[[6-[3-(3-hydroxy-6,8-dioxabicyclo[3.2.1] octanyl)]-2-pyridyl]methoxy]naphthalene). Compound 3g inhibits 5-HPETE production by human 5-LO and LTB4 biosynthesis by human PMN leukocytes and human whole blood (IC50S of 20, 1.6, and 42 nM, respectively). Derivative 3g is orally active in the rat pleurisy model (inhibition of LTB4, ED50 = 0.3 mg/kg) and in the anesthetized dog model (inhibition of ex vivo whole blood LTB4 and urinary LTE4, ED50 = 0.45 and 0.23 microgram/kg/min, respectively, i.v. infusion). In addition, 3g shows excellent functional activity against ovalbumin-induced dyspnea in rats (60% inhibition at 0.5 mg/kg, 4 h pretreatment) and Ascaris-induced bronchoconstriction in conscious sheep (50% and > 85% inhibition in early and late phases, respectively at 2.5 micrograms/kg/min, i.v. infusion) and, more particularly in the conscious antigen sensitive squirrel monkey model (53% inhibition of the increase in RL and 76% in the decrease of Cdyn, at 0.1 mg/kg, po). In rats and dogs, 3g presents excellent pharmacokinetics (estimated half-lives of 5 and 16 h, respectively) and bioavailabilities (26% and 73% when dosed as its hydrochloride salt at doses of 20 and 10 mg/kg, respectively, in methocel suspension). Based on its overall biological profile, compound 3g has been selected for preclinical animal toxicity studies.
二氧杂双环辛烷基萘腈已被报道为一类强效且非氧化还原型的5-脂氧合酶(5-LO)抑制剂。这些双环衍生物在代谢上比其四氢吡喃基类似物更稳定,但口服吸收不佳。用吡啶环取代萘腈1中的苯环可得到强效且口服吸收良好的抑制剂3g(L-739,010,2-氰基-4-(3-呋喃基)-7-[[6-[3-(3-羟基-6,8-二氧杂双环[3.2.1]辛烷基)]-2-吡啶基]甲氧基]萘)。化合物3g可抑制人5-LO产生5-HPETE以及人中性粒细胞和人全血的白三烯B4(LTB4)生物合成(IC50分别为20、1.6和42 nM)。衍生物3g在大鼠胸膜炎模型(抑制LTB4,ED50 = 0.3 mg/kg)和麻醉犬模型(抑制离体全血LTB4和尿白三烯E4(LTE4),ED50分别为0.45和0.23微克/千克/分钟,静脉输注)中具有口服活性。此外,3g对卵清蛋白诱导的大鼠呼吸困难(0.5 mg/kg预处理4小时时抑制60%)和蛔虫诱导的清醒绵羊支气管收缩(静脉输注2.5微克/千克/分钟时,早期和晚期分别抑制50%和>85%),尤其是在清醒的抗原敏感松鼠猴模型(0.1 mg/kg口服时,抑制气道阻力增加53%和动态顺应性降低76%)中表现出优异的功能活性。在大鼠和犬中,3g具有优异的药代动力学(估计半衰期分别为5和16小时)和生物利用度(以其盐酸盐形式在20和10 mg/kg剂量下以甲基纤维素混悬液给药时,生物利用度分别为26%和73%)。基于其整体生物学特性,化合物3g已被选用于临床前动物毒性研究。