Further transformation of fungal catalyzed transformed metabolite 11β-hydroxy-dianabol into new aromatase inhibitors

Bioorg Chem. 2025 Jan:154:108025. doi: 10.1016/j.bioorg.2024.108025. Epub 2024 Dec 3.

Abstract

Secondary biotransformation of 11β-hydroxy-dianabol (11β,17β-dihydroxy-17α-methylandrost-1,4-dien-3-one) (1), catalyzed by using two fungi Gibberella fujikuroi and Cunninghamella blakesleeana at ambient conditions, was carried out to synthesize its analogues. Transformation of compound 1 with G. fujikuroi yielded a new metabolite, 11β, 17β-dihydroxy-17α-methyl-5β-androst-1-ene-3-one (2), while four new derivatives, 6β, 17β-dihydroxy-17α-methylandrost-1,4-diene-3,11-dione (3), 15α,17β-dihydroxy-17α-methylandrost-1,4-diene-3,11-dione (4), 6β,11β,17β-trihydroxy-17α-methylandrost-1,4-dien-3-one (5), and 7β,11β,17β-trihydroxy-17α-methylandrost-1,4-dien-3-one (6) were obtained by transformation with C. blakesleeana. Compounds 1-6 showed a significant aromatase inhibition with IC50 values in the range of 2.01-3.13 μM as compared to the standard drug, exemestane (IC50 = 0.21 ± 0.16 μM). Aromatase is a valid target for drug discovery against ER+ breast cancers. Compounds 1-6 were subjected to molecular docking studies to predict the key interactions, and the MMGBSA studies to analyze the binding affinity and thermal stability of the protein-ligand complexes. Further, the relationship between the metabolites 1-6 and breast tumor androgen receptors was evaluated by in silico approach to analyze the binding interactions between androgen receptors and metabolites. Moreover, compounds 1-6 were found as non-cytotoxic to BJ (Human fibroblast) normal cell line. Hence, these molecules can be further studied for optimization as potential aromatase inhibitors against breast cancer.

Keywords: 11β-Hydroxy-dianabol; Aromatase inhibition; Biocatalytic transformation; Cunninghamella blakesleeana; ER+ breast cancer; Gibberella fujikuroi.

MeSH terms

  • Androstenediols / chemistry
  • Androstenediols / metabolism
  • Androstenediols / pharmacology
  • Antineoplastic Agents / chemical synthesis
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / pharmacology
  • Aromatase Inhibitors* / chemical synthesis
  • Aromatase Inhibitors* / chemistry
  • Aromatase Inhibitors* / pharmacology
  • Aromatase* / metabolism
  • Biocatalysis
  • Biotransformation
  • Cell Proliferation / drug effects
  • Cunninghamella* / metabolism
  • Dose-Response Relationship, Drug
  • Drug Screening Assays, Antitumor
  • Gibberella / drug effects
  • Gibberella / metabolism
  • Humans
  • Molecular Docking Simulation
  • Molecular Structure
  • Structure-Activity Relationship

Substances

  • Aromatase Inhibitors
  • Aromatase
  • Antineoplastic Agents
  • Androstenediols