title: A High-Energy Charge-Separated State of 1.70 eV from a High-Potential Donor-Acceptor Dyad: A Catalyst for Energy-Demanding Photochemical Reactions.
abstract: A high potential donor-acceptor dyad composed of zinc porphyrin bearing three meso-pentafluorophenyl substituents covalently linked to C60 , as a novel dyad capable of generating charge-separated states of high energy (potential) has been developed. The calculated energy of the charge-separated state was found to be 1.70 eV, the highest reported for a covalently linked porphyrin-fullerene dyad. Intramolecular photoinduced electron transfer leading to charge-separated states of appreciable lifetimes in polar and nonpolar solvents has been established from studies involving femto- to nanosecond transient absorption techniques. The high energy stored in the form of charge-separated states along with its persistence of about 50-60 ns makes this dyad a potential electron-transporting catalyst to carry out energy-demanding photochemical reactions. This type of high-energy harvesting dyad is expected to open new research in the areas of artificial photosynthesis especially producing energy (potential) demanding light-to-fuel products.
authors: Department of Chemistry, University of North Texas, 1155 Union Circle, #305070, Denton, TX, 76203-5017, USA.
authors: Gary N
authors: GN
authors: Lim
authors: Department of Chemistry, University of North Texas, 1155 Union Circle, #305070, Denton, TX, 76203-5017, USA.
authors: Christopher O
authors: CO
authors: Obondi
authors: Department of Chemistry, University of North Texas, 1155 Union Circle, #305070, Denton, TX, 76203-5017, USA. Francis.DSouza@UNT.edu.
authors: Francis
authors: 0000-0003-3815-8949
authors: F
authors: D'Souza
keywords: advanced photocatalyst; charge-separated states; donor-acceptor dyad; fluorinated porphyrin; fullerene