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Activationless Multiple-Site Concerted Proton-Electron Tunneling
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- Bowring, Miriam A. (author)
- Yale Univ, Dept Chem, 225 Prospect St, New Haven, CT 06520 USA;Univ Washington, Dept Chem, Seattle, WA 98195 USA;Reed Coll, Dept Chem, Portland, OR 97202 USA
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- Bradshaw, Liam R. (author)
- Univ Washington, Dept Chem, Seattle, WA 98195 USA
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- Parada, Giovanny A. (author)
- Yale Univ, Dept Chem, 225 Prospect St, New Haven, CT 06520 USA
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- (creator_code:org_t)
- 2018-05-30
- 2018
- English.
- In: Journal of the American Chemical Society. - : AMER CHEMICAL SOC. - 0002-7863 .- 1520-5126. ; 140:24, s. 7449-7452
- Journal article (peer-reviewed)
Abstract
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- 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 photo-induced 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 X 10(10) 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.
Subject headings
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
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- art (subject category)
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