Brand Stephen, Norcross Neil R, Thompson Stephen, Harrison Justin R, Smith Victoria C, Robinson David A, Torrie Leah S, McElroy Stuart P, Hallyburton Irene, Norval Suzanne, Scullion Paul, Stojanovski Laste, Simeons Frederick R C, van Aalten Daan, Frearson Julie A, Brenk Ruth, Fairlamb Alan H, Ferguson Michael A J, Wyatt Paul G, Gilbert Ian H, Read Kevin D
Drug Discovery Unit, Division of Biological Chemistry and Drug Discovery, College of Life Sciences, University of Dundee , Sir James Black Centre, Dundee DD1 5EH, U.K.
J Med Chem. 2014 Dec 11;57(23):9855-69. doi: 10.1021/jm500809c. Epub 2014 Nov 20.
Trypanosoma brucei N-myristoyltransferase (TbNMT) is an attractive therapeutic target for the treatment of human African trypanosomiasis (HAT). From previous studies, we identified pyrazole sulfonamide, DDD85646 (1), a potent inhibitor of TbNMT. Although this compound represents an excellent lead, poor central nervous system (CNS) exposure restricts its use to the hemolymphatic form (stage 1) of the disease. With a clear clinical need for new drug treatments for HAT that address both the hemolymphatic and CNS stages of the disease, a chemistry campaign was initiated to address the shortfalls of this series. This paper describes modifications to the pyrazole sulfonamides which markedly improved blood-brain barrier permeability, achieved by reducing polar surface area and capping the sulfonamide. Moreover, replacing the core aromatic with a flexible linker significantly improved selectivity. This led to the discovery of DDD100097 (40) which demonstrated partial efficacy in a stage 2 (CNS) mouse model of HAT.
布氏锥虫N-肉豆蔻酰基转移酶(TbNMT)是治疗人类非洲锥虫病(HAT)的一个有吸引力的治疗靶点。根据以往的研究,我们鉴定出吡唑磺酰胺DDD85646(1),一种有效的TbNMT抑制剂。尽管该化合物是一个很好的先导化合物,但中枢神经系统(CNS)暴露不足限制了其仅用于该疾病的血淋巴期(1期)。鉴于临床上明确需要针对HAT的新药物治疗方法,以解决该疾病的血淋巴期和CNS期问题,于是开展了一项化学研究活动来解决该系列药物的不足。本文描述了对吡唑磺酰胺的修饰,通过减少极性表面积和封闭磺酰胺基团,显著提高了血脑屏障通透性。此外,用柔性连接子取代核心芳香环显著提高了选择性。这导致发现了DDD100097(40),其在HAT的2期(CNS)小鼠模型中显示出部分疗效。