Two-Channel Model for Electron Transfer in a Dye-Catalyst-Dye Supramolecular Complex for Photocatalytic Water Splitting.

ChemSusChem
YangFrancesco Buda

Abstract

To improve the performance of dye-sensitized photoelectrochemical cell (DS-PEC) devices for splitting water, the tailoring of the photocatalytic four-photon water oxidation half-reaction represents a principle challenge of fundamental significance. In this study, a Ru-based water oxidation catalyst (WOC) covalently bound to two 2,6-diethoxy-1,4,5,8-diimide-naphthalene (NDI) dye functionalities provides comparable driving forces and channels for electron transfer. Constrained ab initio molecular dynamics simulations are performed to investigate the photocatalytic cycle of this two-channel model for photocatalytic water splitting. The introduction of a second light-harvesting dye in the Ru-based dye-WOC-dye supramolecular complex enables two separate parallel electron-transfer channels, leading to a five-step catalytic cycle with three intermediates and two doubly oxidized states. The total spin S=1 is conserved during the catalytic process and the system with opposite spin on the oxidized NDI proceeds from the Ru=O intermediate to the final Ru-O2 intermediate with a triplet molecular 3 O2 ligand that is eventually released into the environment. The in-depth insight into the proposed photocatalytic cycle of the two-channel model ...Continue Reading

References

Jun 1, 1970·Photochemistry and Photobiology·B KokM McGloin
Nov 20, 2001·Nature·M Grätzel
Apr 20, 2007·Journal of the American Chemical Society·André R GroenhofKoop Lammertsma
Sep 17, 2008·The Journal of Physical Chemistry. B·Francesca Costanzo, Raffaele Guido Della Valle
Apr 3, 2010·Proceedings of the National Academy of Sciences of the United States of America·Zuofeng ChenThomas J Meyer
Dec 15, 2010·Chemical Reviews·Sharon Hammes-Schiffer
Jan 9, 2012·Chemphyschem : a European Journal of Chemical Physics and Physical Chemistry·José Luis Vallés-PardoFrancesco Buda
Apr 25, 2012·Proceedings of the National Academy of Sciences of the United States of America·Samantha HorvathSharon Hammes-Schiffer
Oct 20, 2012·Chemical Society Reviews·John R Swierk, Thomas E Mallouk
Mar 13, 2013·Proceedings of the National Academy of Sciences of the United States of America·Simone PiccininStefano Fabris
Jan 28, 2014·Journal of Chemical Information and Modeling·Alexandra T P Carvalho, Marcel Swart
Jan 30, 2014·Chemical Society Reviews·Serena BerardiAntoni Llobet
Apr 16, 2014·Inorganic Chemistry·Brian H Solis, Sharon Hammes-Schiffer
Apr 8, 2015·Proceedings of the National Academy of Sciences of the United States of America·Na SongThomas J Meyer
May 20, 2015·Journal of the American Chemical Society·Pablo Garrido-BarrosAntoni Llobet
Jun 26, 2015·Journal of the American Chemical Society·Sharon Hammes-Schiffer
Aug 1, 2015·Journal of the American Chemical Society·Roc MatheuAntoni Llobet
Aug 27, 2016·Chemical Reviews·Mohammad Al KobaisiSheshanath V Bhosale
Sep 23, 2016·Journal of the American Chemical Society·M Kyle BrennamanThomas J Meyer
Jun 20, 2018·Proceedings of the National Academy of Sciences of the United States of America·Pengtao XuThomas E Mallouk
Aug 8, 2018·Proceedings of the National Academy of Sciences of the United States of America·Degao WangThomas J Meyer
May 24, 2019·Chemical Society Reviews·Sining YunAnders Hagfeldt
Mar 26, 2020·Journal of Chemical Theory and Computation·Mauro SchillingSandra Luber
Jul 11, 2020·The Journal of Physical Chemistry. a·Jelena BelićLucas Visscher

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Citations

Dec 9, 2021·Physical Chemistry Chemical Physics : PCCP·Jelena BelićLucas Visscher

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