TY - JOUR
T1 - Integrating photoconversion building blocks with catalysts for solar fuels formation
AU - Wasielewski, Michael R.
AU - Samuel, Amanda P S
AU - Co, Dick T.
AU - Stern, Charlotte L.
PY - 2010/12/1
Y1 - 2010/12/1
N2 - We will report on electron transfer dynamics in several photodriven charge separation systems covalently-linked at fixed distances to catalysts for solar fuels formation. For example, the synthesis and spectroscopic characterization of a naphthalene-4,5-dicarboximide-1,8-dithiolate diiron complex (NMI-Fe2S2(CO)6, 1) and a covalently-linked, fixed-distance zinc 5,10,15-tri-n-pentyl-20-phenylporphyrin-NMI-Fe2S2(CO)6 donor-acceptor dyad (2) will be discussed. The electron-withdrawing nature of the NMI group makes the diiron complex among the most easily reduced hydrogenase mimics (-0.74 V vs. SCE) reported to date. Selective photoexcitation of the Zn porphyrin in 2 with 553 nm, 110-fs laser pulses yields transient absorption spectra in CH2Cl2 that show a distinct peak at 616 nm, which is assigned to (NMI-Fe2S2(CO)6)-• based on spectroelectrochemical measurements on 1, and is used to monitor the charge separation (CS) and charge recombination (CR) dynamics of 2.
AB - We will report on electron transfer dynamics in several photodriven charge separation systems covalently-linked at fixed distances to catalysts for solar fuels formation. For example, the synthesis and spectroscopic characterization of a naphthalene-4,5-dicarboximide-1,8-dithiolate diiron complex (NMI-Fe2S2(CO)6, 1) and a covalently-linked, fixed-distance zinc 5,10,15-tri-n-pentyl-20-phenylporphyrin-NMI-Fe2S2(CO)6 donor-acceptor dyad (2) will be discussed. The electron-withdrawing nature of the NMI group makes the diiron complex among the most easily reduced hydrogenase mimics (-0.74 V vs. SCE) reported to date. Selective photoexcitation of the Zn porphyrin in 2 with 553 nm, 110-fs laser pulses yields transient absorption spectra in CH2Cl2 that show a distinct peak at 616 nm, which is assigned to (NMI-Fe2S2(CO)6)-• based on spectroelectrochemical measurements on 1, and is used to monitor the charge separation (CS) and charge recombination (CR) dynamics of 2.
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M3 - Conference article
AN - SCOPUS:79951471359
SN - 0065-7727
JO - ACS National Meeting Book of Abstracts
JF - ACS National Meeting Book of Abstracts
T2 - 240th ACS National Meeting and Exposition
Y2 - 22 August 2010 through 26 August 2010
ER -