Activationless Multiple-Site Concerted Proton-Electron Tunneling

Journal of the American Chemical Society
Miriam A BowringJames M Mayer

Abstract

The transfer of protons and electrons is key to energy conversion and storage, from photosynthesis to fuel cells. Increased understanding and control of these processes are needed. A new anthracene-phenol-pyridine molecular triad was designed to undergo fast photoinduced multiple-site concerted proton-electron transfer (MS-CPET), with the phenol moiety transferring an electron to the photoexcited anthracene and a proton to the pyridine. Fluorescence quenching and transient absorption experiments in solutions and glasses show rapid MS-CPET (3.2 × 1010 s-1 at 298 K). From 5.5 to 90 K, the reaction rate and kinetic isotope effect (KIE) are independent of temperature, with zero Arrhenius activation energy. From 145 to 350 K, there are only slight changes with temperature. This MS-CPET reaction thus occurs by tunneling of both the proton and electron, in different directions. Since the reaction proceeds without significant thermal activation energy, the rate constant indicates the magnitude of the electron/proton double tunneling probability.

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Citations

Feb 28, 2019·Chemical Communications : Chem Comm·Andrea Pannwitz, Oliver S Wenger
Apr 25, 2019·Faraday Discussions·Zachary K GoldsmithSharon Hammes-Schiffer
Oct 2, 2020·Physical Chemistry Chemical Physics : PCCP·Zong-Ying LiuPi-Tai Chou
Dec 20, 2018·Dalton Transactions : an International Journal of Inorganic Chemistry·Andrea Pannwitz, Oliver S Wenger
Apr 13, 2019·Science·Giovanny A ParadaJames M Mayer
Mar 3, 2020·Chemical Science·Wesley B SwordsLeif Hammarström
Dec 18, 2019·Journal of the American Chemical Society·Elvira R Sayfutyarova, Sharon Hammes-Schiffer
Nov 1, 2018·Journal of the American Chemical Society·Emmanuel OdellaAna L Moore
Aug 26, 2021·The Journal of Physical Chemistry. a·Laura F CotterLeif Hammarström
Aug 14, 2020·The Journal of Physical Chemistry Letters·Elvira R Sayfutyarova, Sharon Hammes-Schiffer
Jun 9, 2020·Journal of the American Chemical Society·Brian KoronkiewiczJames M Mayer
Nov 4, 2020·Journal of the American Chemical Society·Jenny Y YangJeffrey M Barlow

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