Dipartimento di Chimica "Ugo Schiff" DICUS, Università di Firenze, Via della Lastruccia 3-13, 50019, Sesto, Fiorentino (FI), Italy.
Dipartimento di Scienze Biomediche, Sperimentali e Cliniche Mario Serio, Università di Firenze, Viale Morgagni 50, 50134, Firenze, Italy.
Chembiochem. 2022 Jun 3;23(11):e202200077. doi: 10.1002/cbic.202200077. Epub 2022 Apr 7.
The synthesis of five new multivalent derivatives of a trihydroxypiperidine iminosugar was accomplished through copper catalyzed alkyne-azide cycloaddition (CuAAC) reaction of an azido ending piperidine and several propargylated scaffolds. The resulting multivalent architectures were assayed as inhibitors of lysosomal GCase, the defective enzyme in Gaucher disease. The multivalent compounds resulted in much more potent inhibitors than a parent monovalent reference compound, thus showing a good multivalent effect. Biological investigation of these compounds as pharmacological chaperones revealed that the trivalent derivative (12) gives a 2-fold recovery of the GCase activity on Gaucher patient fibroblasts bearing the L444P/L444P mutations responsible for neuropathies. Additionally, a thermal denaturation experiment showed its ability to impart stability to the recombinant enzyme used in therapy.
通过铜催化的叠氮化物-炔烃环加成(CuAAC)反应,将末端叠氮化物的哌啶与几种丙炔基支架连接,合成了五新的三羟基哌啶亚氨基糖的多价衍生物。将所得的多价结构作为溶酶体 GCase 的抑制剂进行了测定,GCase 是 Gaucher 病中缺陷的酶。与母体单价参比化合物相比,多价化合物的抑制效果要强得多,因此表现出良好的多价效应。作为药理学伴侣对这些化合物的生物学研究表明,三价衍生物(12)可使携带导致神经病变的 L444P/L444P 突变的 Gaucher 病患者成纤维细胞中的 GCase 活性恢复两倍。此外,热变性实验表明其能够赋予治疗中使用的重组酶以稳定性。