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Concerted proton-el...
Concerted proton-electron transfer reactions in the Marcus inverted region
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- Parada, Giovanny A. (författare)
- Yale Univ, Dept Chem, New Haven, CT 06520 USA
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- Goldsmith, Zachary K. (författare)
- Yale Univ, Dept Chem, New Haven, CT 06520 USA
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- Kolmar, Scott (författare)
- Yale Univ, Dept Chem, New Haven, CT 06520 USA
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- Pettersson-Rimgard, Belinda (författare)
- Uppsala universitet,Fysikalisk kemi
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- Mercado, Brandon Q. (författare)
- Yale Univ, Dept Chem, New Haven, CT 06520 USA
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- Hammarström, Leif, 1964- (författare)
- Uppsala universitet,Fysikalisk kemi
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- Hammes-Schiffer, Sharon (författare)
- Yale Univ, Dept Chem, New Haven, CT 06520 USA
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- Mayer, James M. (författare)
- Yale Univ, Dept Chem, New Haven, CT 06520 USA
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(creator_code:org_t)
- American Association for the Advancement of Science (AAAS), 2019
- 2019
- Engelska.
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 364:6439, s. 471-475
- Relaterad länk:
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https://europepmc.or...
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https://urn.kb.se/re...
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https://doi.org/10.1...
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Abstract
Ämnesord
Stäng
- Electron transfer reactions slow down when they become very thermodynamically favorable, a counterintuitive interplay of kinetics and thermodynamics termed the inverted region in Marcus theory. Here we report inverted region behavior for proton-coupled electron transfer (PCET). Photochemical studies of anthracene-phenol-pyridine triads give rate constants for PCET charge recombination that are slower for the more thermodynamically favorable reactions. Photoexcitation forms an anthracene excited state that undergoes PCET to create a charge-separated state. The rate constants for return charge recombination show an inverted dependence on the driving force upon changing pyridine substituents and the solvent. Calculations using vibronically nonadiabatic PCET theory yield rate constants for simultaneous tunneling of the electron and proton that account for the results.
Ämnesord
- NATURVETENSKAP -- Kemi -- Fysikalisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Physical Chemistry (hsv//eng)
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