Discovery of novel BCR-ABL PROTACs based on the cereblon E3 ligase design, synthesis, and biological evaluation

  • Eur J Med Chem. 2021 Nov 5:223:113645. doi: 10.1016/j.ejmech.2021.113645.
Haixia Liu  1 Xinyu Ding  2 Linyi Liu  3 Qianglong Mi  4 Quanju Zhao  5 YuBao Shao  6 Chaowei Ren  4 Jinju Chen  5 Ying Kong  5 Xing Qiu  7 Nicola Elvassore  5 Xiaobao Yang  8 Qianqian Yin  9 Biao Jiang  10
Affiliations
  • 1. School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210, China; Shanghai Institute for Advanced Immunochemical Studies, China; University of Chinese Academy of Sciences, Beijing, 100049, China.
  • 2. Shanghai Institute for Advanced Immunochemical Studies, China; School of Life Science and Technology, China; University of Chinese Academy of Sciences, Beijing, 100049, China.
  • 3. Hunan Provincial Key Laboratory of Tumor Microenvironment Responsive Drug Research, School of Pharmaceutical Science, University of South China, Hengyang City, 421001, China.
  • 4. Shanghai Institute for Advanced Immunochemical Studies, China; School of Life Science and Technology, China.
  • 5. Shanghai Institute for Advanced Immunochemical Studies, China.
  • 6. Department of Histology and Embryology, Anhui Medical University, Hefei, 230032, China.
  • 7. CAS Key Laboratory of Synthetic Chemistry of Natural Substances, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, 345 Lingling Road, Shanghai, 200032, China.
  • 8. Shanghai Institute for Advanced Immunochemical Studies, China. Electronic address: [email protected].
  • 9. Shanghai Institute for Advanced Immunochemical Studies, China. Electronic address: [email protected].
  • 10. Shanghai Institute for Advanced Immunochemical Studies, China; CAS Key Laboratory of Synthetic Chemistry of Natural Substances, Shanghai Institute of Organic Chemistry, Chinese Academy of Sciences, 345 Lingling Road, Shanghai, 200032, China. Electronic address: [email protected].
Abstract

Protein degradation is a promising strategy for drug development. Proteolysis-targeting chimeras (PROTACs) hijacking the E3 ligase Cereblon (CRBN) exhibit enormous potential and universal degradation performance due to the small molecular weight of CRBN ligands. In this study, the CRBN-recruiting PROTACs were explored on the degradation of oncogenic fusion protein Bcr-Abl, which drives the pathogenesis of chronic myeloid leukemia (CML). A series of novel PROTACs were synthesized by conjugating Bcr-Abl Inhibitor dasatinib to the CRBN ligand including pomalidomide and lenalidomide, and the extensive structure-activity relationship (SAR) studies were performed focusing on optimization of linker parameters. Therein, we uncovered that pomalidomide-based degrader 17 (SIAIS056), possessing sulfur-substituted carbon chain linker, exhibits the most potent degradative activity in vitro and favorable pharmacokinetics in vivo. Besides, degrader 17 also degrades a variety of clinically relevant resistance-conferring mutations of Bcr-Abl. Furthermore, degrader 17 induces significant tumor regression against K562 xenograft tumors. Our study indicates that 17 as an efficacious Bcr-Abl degrader warrants intensive investigation for the future treatment of Bcr-Abl+ leukemia.

Keywords
BCR-ABL; CRBN; Degradation; Leukemia; PROTAC.