Histidine-conjugated poly(amino acid) derivatives for the novel endosomolytic delivery carrier of doxorubicin

J Control Release. 2006 Aug 10;114(1):60-8. doi: 10.1016/j.jconrel.2006.05.016. Epub 2006 May 25.

Abstract

Direct conjugation of histidine to poly(2-hydroxyethyl aspartamide) (PHEA-His) and C18-grafted PHEA (PHEA-g-C18-His) was achieved via an ester linkage using N(alpha)-Boc-L-histidine, followed by the deprotection of Boc groups. PHEA-His series would be expected as an endosomolytic synthetic polymer because of the buffering capacity at physiological and endosomal pH regulated by alpha-amine and imidazole groups in side chains. PHEA-g-C18-His series formed stable self-aggregates due to the hydrophobic interaction between grafted alkyl chains. The size, zeta potential, and micropolarity of PHEA-g-C18-His series greatly increased at pH 5.0, because aggregates swelled by a positive surface charge and the electrostatic repulsion of ionized histidine moieties in the aggregate surface. In the confocal microscopy, it was revealed that PHEA-g-C18-His was more uniformly distributed than PHEA-g-C18 in HeLa cells after 8 h of incubation and was attributed to the endosomolytic ability of conjugated histidine moieties. In doxorubicin-loaded self-aggregate systems, the histidine conjugation improved the cell cytotoxicity by a fast release of loaded doxorubicin at low pH and the endosomolytic ability of conjugated histidine, resulting in the easy nuclear access of doxorubicin.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Amines / chemistry
  • Buffers
  • Cell Survival / drug effects
  • Doxorubicin / administration & dosage
  • Doxorubicin / chemistry
  • Doxorubicin / pharmacokinetics*
  • Drug Carriers / administration & dosage
  • Drug Carriers / chemistry
  • Drug Carriers / pharmacokinetics*
  • Endocytosis
  • Endosomes / metabolism*
  • HeLa Cells
  • Histidine / chemistry*
  • Humans
  • Hydrogen-Ion Concentration
  • Magnetic Resonance Spectroscopy
  • Microscopy, Confocal
  • Molecular Structure
  • Particle Size
  • Peptides / chemistry*
  • Spectrum Analysis
  • Static Electricity
  • Surface Properties

Substances

  • Amines
  • Buffers
  • Drug Carriers
  • Peptides
  • alpha,beta-poly((2-hydroxyethyl)-aspartamide)
  • Histidine
  • Doxorubicin
  • stearylamine