Rowbottom Martin W, Bain Gretchen, Calderon Imelda, Lasof Taylor, Lonergan David, Lai Andiliy, Huang Fei, Darlington Janice, Prodanovich Patricia, Santini Angelina M, King Christopher D, Goulet Lance, Shannon Kristen E, Ma Gina L, Nguyen Katherine, MacKenna Deidre A, Evans Jilly F, Hutchinson John H
PharmAkea Therapeutics , San Diego Science Center, 3030 Bunker Hill Street, Suite 300, San Diego, California 92109, United States.
J Med Chem. 2017 May 25;60(10):4403-4423. doi: 10.1021/acs.jmedchem.7b00345. Epub 2017 May 15.
LOXL2 catalyzes the oxidative deamination of ε-amines of lysine and hydroxylysine residues within collagen and elastin, generating reactive aldehydes (allysine). Condensation with other allysines or lysines drives the formation of inter- and intramolecular cross-linkages, a process critical for the remodeling of the ECM. Dysregulation of this process can lead to fibrosis, and LOXL2 is known to be upregulated in fibrotic tissue. Small-molecules that directly inhibit LOXL2 catalytic activity represent a useful option for the treatment of fibrosis. Herein, we describe optimization of an initial hit 2, resulting in identification of racemic-trans-(3-((4-(aminomethyl)-6-(trifluoromethyl)pyridin-2-yl)oxy)phenyl)(3-fluoro-4-hydroxypyrrolidin-1-yl)methanone 28, a potent irreversible inhibitor of LOXL2 that is highly selective over LOX and other amine oxidases. Oral administration of 28 significantly reduced fibrosis in a 14-day mouse lung bleomycin model. The (R,R)-enantiomer 43 (PAT-1251) was selected as the clinical compound which has progressed into healthy volunteer Phase 1 trials, making it the "first-in-class" small-molecule LOXL2 inhibitor to enter clinical development.
赖氨酰氧化酶2(LOXL2)催化胶原蛋白和弹性蛋白中赖氨酸和羟赖氨酸残基的ε-胺的氧化脱氨反应,生成反应性醛(烯赖氨酸)。与其他烯赖氨酸或赖氨酸的缩合驱动分子间和分子内交联的形成,这是细胞外基质重塑的关键过程。该过程的失调可导致纤维化,并且已知LOXL2在纤维化组织中上调。直接抑制LOXL2催化活性的小分子是治疗纤维化的有用选择。在此,我们描述了对初始活性化合物2的优化,从而鉴定出外消旋反式-(3-((4-(氨基甲基)-6-(三氟甲基)吡啶-2-基)氧基)苯基)(3-氟-4-羟基吡咯烷-1-基)甲酮28,一种有效的LOXL2不可逆抑制剂,对赖氨酰氧化酶(LOX)和其他胺氧化酶具有高度选择性。在14天的小鼠肺博来霉素模型中口服28可显著减轻纤维化。(R,R)-对映体43(PAT-1251)被选为临床化合物,已进入健康志愿者1期试验,使其成为进入临床开发的“同类首创”小分子LOXL2抑制剂。