Permanent URL to this publication: http://dx.doi.org/10.5167/uzh-36017
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.
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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.
|Item Type:||Journal Article, refereed, original work|
|Communities & Collections:||07 Faculty of Science > Institute of Physical Chemistry|
|Deposited On:||23 Dec 2010 11:17|
|Last Modified:||02 Dec 2013 18:34|
|Publisher:||National Academy of Sciences|
|Free access at:||Publisher DOI. An embargo period may apply.|
|Other Identification Number:||ISI:000275714300008|
|Citations:||Web of Science®. Times cited: 40|
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