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Barrier-Lowering Effects of Baird Antiaromaticity in Photoinduced Proton-Coupled Electron Transfer (PCET) Reactions.
Karas, Lucas J; Wu, Chia-Hua; Wu, Judy I.
Afiliación
  • Karas LJ; Department of Chemistry, University of Houston, Houston, Texas 77204, United States.
  • Wu CH; Department of Chemistry, University of Houston, Houston, Texas 77204, United States.
  • Wu JI; Department of Chemistry, University of Houston, Houston, Texas 77204, United States.
J Am Chem Soc ; 143(43): 17970-17974, 2021 11 03.
Article en En | MEDLINE | ID: mdl-34672631
Many popular organic chromophores that catalyze photoinduced proton-coupled electron transfer (PCET) reactions are aromatic in the ground state but become excited-state antiaromatic in the lowest ππ* state. We show that excited-state antiaromaticity makes electron transfer easier. Two representative photoinduced electron transfer processes are investigated: (1) the photolysis of phenol and (2) solar water splitting of a pyridine-water complex. In the selected reactions, the directions of electron transfer are opposite, but the net result is proton transfer following the direction of electron transfer. Nucleus-independent chemical shifts (NICS), ionization energies, electron affinities, and PCET energy profiles of selected [4n] and [4n + 2] π-systems are presented, and important mechanistic implications are discussed.
Asunto(s)

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Piridinas / Agua / Fenol / Electrones Idioma: En Revista: J Am Chem Soc Año: 2021 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Piridinas / Agua / Fenol / Electrones Idioma: En Revista: J Am Chem Soc Año: 2021 Tipo del documento: Article País de afiliación: Estados Unidos Pais de publicación: Estados Unidos