Crystal Pharmatech Co., Ltd. , Suzhou 215123, P.R. China.
Department of Molecular and Medical Pharmacology, University of California , Los Angeles, California 90095, United States.
J Med Chem. 2017 Nov 9;60(21):8847-8857. doi: 10.1021/acs.jmedchem.7b00971. Epub 2017 Oct 19.
Currently, no effective and safe medicines are available to treat diabetic nephropathy (DN). Bardoxolone methyl (CDDO-Me) has displayed promising anti-DN activity as well as serious side effects in clinical trials, probably because the highly reactive α-cyano-α,β-unsaturated ketone (CUK) in ring A of CDDO-Me can covalently bind to thiol functionalities in many biomacromolecules. In this study, we designed and synthesized a γ-glutamyl transpeptidase (GGT)-based and CUK-modified derivative of CDDO-Me (2) to address this issue. 2 can be specifically cleaved by GGT, which is highly expressed in the kidney, to liberate CDDO-Me in situ. It should be noted that 2 exhibited anti-DN efficacy comparable to that of CDDO-Me with much less toxicity in cells and db/db mice, suggesting that its safety is better than CDDO-Me. Our findings not only reveal the therapeutic potential of 2 but also provide a strategy to optimize other synthetic molecules or natural products bearing a pharmacophore like CUK to achieve safer pharmaceutical drugs.
目前,尚无有效且安全的药物可用于治疗糖尿病肾病(DN)。在临床试验中,Bardoxolone 甲基(CDDO-Me)表现出有前景的抗 DN 活性,但也有严重的副作用,这可能是因为 CDDO-Me 环 A 中的高反应性α-氰基-α,β-不饱和酮(CUK)可以与许多生物大分子中的巯基功能基团共价结合。在这项研究中,我们设计并合成了基于γ-谷氨酰转肽酶(GGT)和 CUK 修饰的 CDDO-Me 衍生物(2)来解决这个问题。2 可以被高度表达在肾脏中的 GGT 特异性切割,从而原位释放 CDDO-Me。值得注意的是,2 在细胞和 db/db 小鼠中表现出与 CDDO-Me 相当的抗 DN 功效,但毒性要小得多,这表明其安全性优于 CDDO-Me。我们的研究结果不仅揭示了 2 的治疗潜力,还为优化其他含有类似 CUK 药效团的合成分子或天然产物提供了一种策略,以实现更安全的药物。