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Target-Agnostic P-Glycoprotein Assessment Yields Strategies to Evade Efflux, Leading to a BRAF Inhibitor with Intracranial Efficacy.
Kelly, Aya M; Berry, Matthew R; Tasker, Sarah Z; McKee, Sydney A; Fan, Timothy M; Hergenrother, Paul J.
Afiliación
  • Kelly AM; Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.
  • Berry MR; Carl R. Woese Institute for Genomic Biology, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.
  • Tasker SZ; Department of Veterinary Clinical Medicine, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.
  • McKee SA; Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.
  • Fan TM; Carl R. Woese Institute for Genomic Biology, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.
  • Hergenrother PJ; Department of Chemistry, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States.
J Am Chem Soc ; 144(27): 12367-12380, 2022 07 13.
Article en En | MEDLINE | ID: mdl-35759775
The blood-brain barrier (BBB) presents a major hurdle in the development of central nervous system (CNS) active therapeutics, and expression of the P-glycoprotein (P-gp) efflux transporter at the blood-brain interface further impedes BBB penetrance of most small molecules. Designing efflux liabilities out of compounds can be laborious, and there is currently no generalizable approach to directly transform periphery-limited agents to ones active in the CNS. Here, we describe a target-agnostic, prospective assessment of P-gp efflux using diverse compounds. Our results demonstrate that reducing the molecular size or appending a carboxylic acid in many cases enables evasion of P-gp efflux in cell-based experiments and in mice. These strategies were then applied to transform a periphery-limited V600EBRAF inhibitor, dabrafenib, into versions that possess potent and selective anti-cancer activity but now also evade P-gp-mediated efflux. When compared to dabrafenib, the compound developed herein (everafenib) has superior BBB penetrance and superior efficacy in an intracranial mouse model of metastatic melanoma, suggesting it as a lead candidate for the treatment of melanoma metastases to the brain and gliomas with BRAF mutation. More generally, the results described herein suggest the actionability of the trends observed in these target-agnostic efflux studies and provide guidance for the conversion of non-BBB-penetrant drugs into versions that are BBB-penetrant and efficacious.
Asunto(s)

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Proteínas Proto-Oncogénicas B-raf / Melanoma Tipo de estudio: Guideline / Observational_studies Límite: Animals Idioma: En Revista: J Am Chem Soc Año: 2022 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Proteínas Proto-Oncogénicas B-raf / Melanoma Tipo de estudio: Guideline / Observational_studies Límite: Animals Idioma: En Revista: J Am Chem Soc Año: 2022 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos