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An atomistic picture of the regeneration process in dye sensitized solar cells


Schiffmann, F; VandeVondele, J; Hutter, J; Urakawa, A; Wirz, R; Baiker, A (2010). An atomistic picture of the regeneration process in dye sensitized solar cells. Proceedings of the National Academy of Sciences of the United States of America (PNAS), 107(11):4830-4833.

Abstract

A highly efficient mechanism for the regeneration of the cis-bis(isothiocyanato) bis(2,2'-bipyridyl-4,4'-dicarboxylato)-ruthenium (II) sensitizing dye (N3) by I- in acetonitrile has been identified by using molecular dynamics simulation based on density functional theory. Barrier-free complex formation of the oxidized dye with both I- and I-2(-), and facile dissociation of I-2(-) and I-3(-) from the reduced dye are key steps in this process. In situ vibrational spectroscopy confirms the reversible binding of I-2 to the thiocyanate group. Additionally, simulations of the electrolyte near the interface suggest that acetonitrile is able to cover the (101) surface of anatase with a passivating layer that inhibits direct contact of the redox mediator with the oxide, and that the solvent structure specifically enhances the concentration of I- at a distance which further favors rapid dye regeneration.

Abstract

A highly efficient mechanism for the regeneration of the cis-bis(isothiocyanato) bis(2,2'-bipyridyl-4,4'-dicarboxylato)-ruthenium (II) sensitizing dye (N3) by I- in acetonitrile has been identified by using molecular dynamics simulation based on density functional theory. Barrier-free complex formation of the oxidized dye with both I- and I-2(-), and facile dissociation of I-2(-) and I-3(-) from the reduced dye are key steps in this process. In situ vibrational spectroscopy confirms the reversible binding of I-2 to the thiocyanate group. Additionally, simulations of the electrolyte near the interface suggest that acetonitrile is able to cover the (101) surface of anatase with a passivating layer that inhibits direct contact of the redox mediator with the oxide, and that the solvent structure specifically enhances the concentration of I- at a distance which further favors rapid dye regeneration.

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Additional indexing

Item Type:Journal Article, refereed, original work
Communities & Collections:07 Faculty of Science > Department of Chemistry
Dewey Decimal Classification:540 Chemistry
Language:English
Date:March 2010
Deposited On:23 Dec 2010 10:17
Last Modified:07 Dec 2017 03:24
Publisher:National Academy of Sciences
ISSN:0027-8424
Free access at:Publisher DOI. An embargo period may apply.
Publisher DOI:https://doi.org/10.1073/pnas.0913277107
Related URLs:http://www.zora.uzh.ch/36766/
Other Identification Number:ISI:000275714300008

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