Hyaluronic Acid-Bilirubin Nanoparticles as a Tumor Microenvironment Reactive Oxygen Species-Responsive Nanomedicine for Targeted Cancer Therapy

Int J Nanomedicine. 2024 May 27:19:4893-4906. doi: 10.2147/IJN.S460468. eCollection 2024.

Abstract

Introduction: The tumor microenvironment (TME) has attracted considerable attention as a potential therapeutic target for cancer. High levels of reactive oxygen species (ROS) in the TME may act as a stimulus for drug release. In this study, we have developed ROS-responsive hyaluronic acid-bilirubin nanoparticles (HABN) loaded with doxorubicin (DOX@HABN) for the specific delivery and release of DOX in tumor tissue. The hyaluronic acid shell of the nanoparticles acts as an active targeting ligand that can specifically bind to CD44-overexpressing tumors. The bilirubin core has intrinsic anti-cancer activity and ROS-responsive solubility change properties.

Methods & results: DOX@HABN showed the HA shell-mediated targeting ability, ROS-responsive disruption leading to ROS-mediated drug release, and synergistic anti-cancer activity against ROS-overproducing CD44-overexpressing HeLa cells. Additionally, intravenously administered HABN-Cy5.5 showed remarkable tumor-targeting ability in HeLa tumor-bearing mice with limited distribution in major organs. Finally, intravenous injection of DOX@HABN into HeLa tumor-bearing mice showed synergistic anti-tumor efficacy without noticeable side effects.

Conclusion: These findings suggest that DOX@HABN has significant potential as a cancer-targeting and TME ROS-responsive nanomedicine for targeted cancer treatment.

Keywords: hyaluronic acid-bilirubin nanomedicine; reactive oxygen species; stimuli-responsive nanomedicine; tumor microenvironment.

MeSH terms

  • Animals
  • Antineoplastic Agents / administration & dosage
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / pharmacokinetics
  • Antineoplastic Agents / pharmacology
  • Bilirubin* / chemistry
  • Bilirubin* / pharmacokinetics
  • Bilirubin* / pharmacology
  • Doxorubicin* / administration & dosage
  • Doxorubicin* / chemistry
  • Doxorubicin* / pharmacokinetics
  • Doxorubicin* / pharmacology
  • Drug Carriers / chemistry
  • Drug Carriers / pharmacokinetics
  • Drug Liberation
  • HeLa Cells
  • Humans
  • Hyaluronan Receptors* / metabolism
  • Hyaluronic Acid* / chemistry
  • Mice
  • Mice, Inbred BALB C
  • Mice, Nude
  • Nanomedicine*
  • Nanoparticles* / chemistry
  • Neoplasms / drug therapy
  • Neoplasms / metabolism
  • Reactive Oxygen Species* / metabolism
  • Tumor Microenvironment* / drug effects
  • Xenograft Model Antitumor Assays

Substances

  • Hyaluronic Acid
  • Reactive Oxygen Species
  • Doxorubicin
  • Hyaluronan Receptors
  • Bilirubin
  • Drug Carriers
  • Antineoplastic Agents

Grants and funding

The Basic Science Research Program through the National Research Foundation of Korea (NRF) funded by the Ministry of Education supported this research (2022M3H4A1A03067401). This research was also supported by a grant of the Korea Health Technology R&D Project through the Korea Health Industry Development Institute (KHIDI), funded by the Ministry of Health & Welfare, Republic of Korea (RS-2023-00265981). A Korea Basic Science Institute (National Research Facilities and Equipment Center) grant funded by the Ministry of Education supported this research (2023R1A6C103A026).