Raig Nicolai D, Surridge Katherine J, Sanz-Murillo Marta, Dederer Verena, Krämer Andreas, Schwalm Martin P, Elson Lewis, Chatterjee Deep, Mathea Sebastian, Hanke Thomas, Leschziner Andres E, Reck-Peterson Samara L, Knapp Stefan
Institute of Pharmaceutical Chemistry, Goethe University, Max-von-Laue-Str. 9, 60438 Frankfurt am Main, Germany.
Structural Genomics Consortium (SGC), Buchmann Institute for Life Sciences, Max-von-Laue-Str. 15, 60438 Frankfurt am Main, Germany.
bioRxiv. 2025 Feb 13:2024.09.17.613365. doi: 10.1101/2024.09.17.613365.
Aberrant increases in kinase activity of leucine-rich repeat kinase 2 (LRRK2) are associated with Parkinson's disease (PD). Numerous LRRK2-selective type-I kinase inhibitors have been developed and some have entered clinical trials. In this study, we present the first LRRK2-selective type-II kinase inhibitors. Targeting the inactive conformation of LRRK2 is functionally distinct from targeting the active-like conformation using type-I inhibitors. We designed these inhibitors using a combinatorial chemistry approach fusing selective LRRK2 type-I and promiscuous type-II inhibitors by iterative cycles of synthesis supported by structural biology and activity testing. Our current lead structures are selective and potent LRRK2 inhibitors. Through cellular assays, cryo-electron microscopy structural analysis, and in vitro motility assays, we show that our inhibitors stabilize the open, inactive kinase conformation. These new conformation-specific compounds will be invaluable as tools to study LRRK2's function and regulation, and expand the potential therapeutic options for PD.
富含亮氨酸重复激酶2(LRRK2)激酶活性的异常增加与帕金森病(PD)相关。众多LRRK2选择性I型激酶抑制剂已被开发出来,其中一些已进入临床试验阶段。在本研究中,我们展示了首个LRRK2选择性II型激酶抑制剂。靶向LRRK2的无活性构象在功能上与使用I型抑制剂靶向活性样构象不同。我们采用组合化学方法,通过由结构生物学和活性测试支持的迭代合成循环,将选择性LRRK2 I型抑制剂和通用II型抑制剂融合,设计出了这些抑制剂。我们目前的先导结构是选择性且强效的LRRK2抑制剂。通过细胞试验、冷冻电镜结构分析和体外运动试验,我们表明我们的抑制剂能稳定开放的、无活性的激酶构象。这些新的构象特异性化合物作为研究LRRK2功能和调节的工具将非常宝贵,并扩展了PD的潜在治疗选择。