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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Temperature dependence of excited-state proton transfer in water electrolyte solutions and water-methanol solutions
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Temperature dependence of excited-state proton transfer in water electrolyte solutions and water-methanol solutions

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摘要

The reversible proton dissociation and geminate recombination of a photoacid is studied as a function of temperature in water electrolyte solutions and binary water-methanol mixtures, containing 0.1 and 0.2 mole fractions of methanol. 8-Hydroxypyrene-1,3,6-trisulfonate trisodium salt ( HPTS) is used as the photoacid. The experimental data are analyzed by the reversible geminate recombination model. We found that the slope of the logarithm of the proton-transfer rate constant as a function of the inverse of temperature (Arrhenius plot) in the liquid phase of these samples are temperature-dependent, while in the solid phase, the slope is nearly constant. The slope of the Arrhenius plot in frozen electrolyte solution is larger than that of the water-methanol mixtures, which is about the same as in pure water. Careful examination of the time-resolved emission in ice samples shows that the fit quality using the geminate recombination model is rather poor at relatively short times. We were able to get a better fit using an inhomogeneous kinetics model assuming the proton-transfer rate consists of a distribution of rates. The model is consistent with an inhomogeneous frozen water distribution next to the photoacid.

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