Synthesis of saxitoxin derivatives bearing guanidine and urea groups at C13 and evaluation of their inhibitory activity on voltage-gated sodium channels

Org Biomol Chem. 2013 Oct 14;11(38):6642-9. doi: 10.1039/c3ob41398e. Epub 2013 Aug 30.

Abstract

Here, we describe the synthesis of the first C13-N-substituted STX derivatives 4, 5, and 6 bearing a guanidine, a urea group, and an acetamide, respectively, via the fully protected saxitoxinol derivative 8. These compounds are of interest because a previous docking study of saxitoxin (STX) with voltage-gated sodium channels (NaVCh) suggested that the C13 carbamoyl group of STX interacts with residue E403 in the pore region of NaVCh. In a cell-based assay with Neuro-2a cells, the NaVCh-inhibitory activities of 4 and 5 were more than 20- to 50-fold weaker than that of decarbamoyl-STX (3), which is 10-fold less potent than STX. On the other hand, 6 was 1000 times less potent than 3. The electrostatic analysis of C13 in STX and its analogs 4-6 using EON calculations suggested that the NaVCh-inhibitory activity of these derivatives is influenced by both the hydrophilicity and the charge balance of the substituent at C13.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Cell Line, Tumor
  • Cell Survival / drug effects
  • Dose-Response Relationship, Drug
  • Guanidine / chemistry*
  • Mice
  • Molecular Structure
  • Saxitoxin / chemical synthesis*
  • Saxitoxin / chemistry
  • Saxitoxin / pharmacology*
  • Structure-Activity Relationship
  • Urea / chemistry*
  • Voltage-Gated Sodium Channels / metabolism*

Substances

  • Voltage-Gated Sodium Channels
  • Saxitoxin
  • Urea
  • Guanidine