Kinetic analysis of nitroxide radical formation under oxygenated photolysis: toward quantitative singlet oxygen topology

Photochem Photobiol Sci. 2014 Dec;13(12):1804-11. doi: 10.1039/c4pp00318g. Epub 2014 Nov 5.

Abstract

Reaction kinetics for two sterically hindered secondary amines with singlet oxygen have been studied in detail. A water soluble porphyrin sensitizer, 5,10,15,20-tetrakis-(4-sulfunatophenyl)-21,23H-porphyrin (TPPS), was irradiated in oxygenated aqueous solutions containing either 2,2,6,6-tetramethylpiperidin-4-one (TMPD) or 4-[N,N,N-trimethyl-ammonium]-2,2,6,6-tetramethylpiperidinyl chloride (N-TMPCl). The resulting sensitization reaction produced singlet oxygen in high yield, ultimately leading to the formation of the corresponding nitroxide free radicals (R2NO) which were detected using steady-state electron paramagnetic resonance (EPR) spectroscopy. Careful actinometry and EPR calibration curves, coupled with a detailed kinetic analysis, led to a simple and compact expression relating the nitroxide quantum yield ΦR2NO (from the doubly-integrated EPR signal intensity) to the initial amine concentration [R2NH]i. With all other parameters held constant, a plot of ΦR2NOvs. [R2NH]i gave a straight line with a slope proportional to the rate constant for nitroxide formation, kR2NO. This establishment of a rigorous quantitative relationship between the EPR signal and the rate constant provides a mechanism for quantifying singlet oxygen production as a function of its topology in heterogeneous media. Implications for in vivo assessment of singlet oxygen topology are briefly discussed.

Publication types

  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Amines / chemistry
  • Electron Spin Resonance Spectroscopy
  • Energy Transfer
  • Kinetics
  • Molecular Structure
  • Nitrogen Oxides / chemistry
  • Photolysis
  • Porphyrins / chemistry
  • Singlet Oxygen / chemistry*
  • Solutions
  • Water / chemistry

Substances

  • Amines
  • Nitrogen Oxides
  • Porphyrins
  • Solutions
  • Water
  • Singlet Oxygen
  • tetraphenylporphine sulfonate
  • nitroxyl