Molecular degraders (esp. PROTACs) are seeing immense interest as new modalities to combat difficult to treat diseases. After the first PROTACs (ARV-110/ARV-471) showed positive phase I/II results in cancer treatments (e.g., NCT03888612), ARV-471 was granted Fast Track designation by the FDA in 02/2024 for monotherapy for ER+/HER2- advanced or metastatic breast cancer.
While the cancer space is exploding with projects on degrader candidates, degraders for neurodegenerative disorders are understudied due to the perceived drug-unlikeness of PROTACs paired with CNS-delivery concerns. However, degrading certain CNS-proteins constitutes a promising therapeutic strategy for dependent proteinopathies. Its translatability is thus worth exploring.1
In this ongoing work, we focus on TDP-43, a nuclear RNA-binding protein that, when translocating to the cytosol, can form neurotoxic aggregates which are correlated with motor neuron disease (>97% of case) and frontotemporal degeneration (~50% of cases).2, 3 Our synthetic campaign starts via a known, moderate-affinity ligand (nTRD22)4 to synthesise PROTACs in a high-throughput format using bioconjugatable moieties on the ligand, the linkers and E3 ligase recruiters. This allows to rapidly generate PROTACs on analytical scale for high-throughput screening in a flow cytometric assay. In parallel, we perform an affinity selection mass spectrometry screening assay against aggregates-on-a-chip that represent the pathological aggregate conformations to identify more avid binders, and map protein-ligand/-PROTAC interactions via native mass spectrometry.
(1) Farrell K., Jarome T. Is PROTAC technology really a game changer for central nervous system drug discovery? Exp Op Drug Disc 2021, 16(8):833
(2) Wilson D. et al. Hallmarks of neurodegenerative diseases. Cell 2023, 186(4):693.
(3) Scheres S. et al. Molecular pathology of neurodegenerative diseases by cryo-EM of amyloids. Nature 2023, 621(7980):701.
(4) Mollasalehi N. et al. An Allosteric Modulator of RNA Binding Targeting the N-Terminal Domain of TDP-43 Yields Neuroprotective Properties. ACS Chem Biol 2020, 15(11):2854.