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Area of Science:

  • Biomedical Engineering
  • Materials Science
  • Chemistry

Background:

  • Photodynamic therapy (PDT) faces challenges due to poor light penetration and low oxygen levels in tumors.
  • Programmable singlet-oxygen batteries (PSOBs) offer a promising solution by storing and releasing singlet oxygen (1O2) independently of light and oxygen.
  • Current methods for tuning PSOB lifetimes are limited, restricting their clinical applicability.

Purpose of the Study:

  • To develop a sterically controlled PSOB strategy for "OFF-ON-OFF" 1O2 release at tumor sites.
  • To enhance the stability and control the release kinetics of PSOBs for improved therapeutic outcomes.
  • To investigate the impact of steric hindrance on the stability of metastable oxygen bridges in PSOBs.

Main Methods:

  • Synthesized SOB-A and SOB-B with linear substitutions at the bridgehead carbon to enhance 1O2 storage.
  • Encapsulated SOB-A and SOB-B in Cu(II)-based MOF-199 to leverage nanoconfinement for increased stability.
  • Utilized MOF-199 as a precursor for Cu(I) in the tumor microenvironment to catalyze in situ synthesis of a sterically hindered PSOB (SOB-AB) for rapid 1O2 release.

Main Results:

  • Linear substitutions increased 1O2 storage half-lives (t1/2) of SOB-A and SOB-B to 10.5 and 8.7 hours, respectively.
  • Nanoconfinement in MOF-199 extended the half-life to approximately 60 hours, ensuring minimal pretherapy side effects.
  • In situ generated SOB-AB rapidly released 1O2 with a t1/2 of 9.5 minutes in the tumor microenvironment.

Conclusions:

  • Steric hindrance significantly impacts the stability of metastable oxygen bridges in PSOBs.
  • The developed sterically controlled PSOB strategy enables tunable 1O2 release for effective photodynamic therapy.
  • This approach paves the way for next-generation PSOBs with maximized efficiency and minimized side effects through dynamic steric effects.