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Effects of Bridging Ligands on the Current−Potential Behavior and Interfacial Kinetics of Ruthenium-Sensitized Nanocrystalline TiO_2 Photoelectrodes

Kilså, Kristine and Mayo, Elizabeth I. and Kuciauskas, Darius and Villahermosa, Randy and Lewis, Nathan S. and Winkler, Jay R. and Gray, Harry B. (2003) Effects of Bridging Ligands on the Current−Potential Behavior and Interfacial Kinetics of Ruthenium-Sensitized Nanocrystalline TiO_2 Photoelectrodes. Journal of Physical Chemistry A, 107 (18). pp. 3379-3383. ISSN 1089-5639. doi:10.1021/jp021921u. https://resolver.caltech.edu/CaltechAUTHORS:20170519-142727736

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Abstract

We have shown that Ru^(II)(bpy)_2(bpy-4-(xylyl)_x-≡-phenyl-COOH)(PF_6)_2 (abbreviated Rux, where x = 0, 1 or 2 xylyl groups; bpy = 2,2‘-bipyridine) dyes can act as sensitizers for nanocrystalline TiO_2 in functional photoelectrochemical cells under simulated solar illumination, albeit with low efficiencies. Both the short-circuit photocurrent density and the open-circuit voltage decreased as x was increased. Electron injection (10^6−10^8 s^(-1)) was slightly faster for the x = 0 dye, but both recombination (10^(-15)−10^(-13) cm^3 s^(-1)) and regeneration (10^4−10^6 s^(-1) for 10 mM I^-) were slightly faster for the x = 2 dye. We suggest that the lack of distance dependence is due to the flexible one-carboxyl attachment to the surface resulting in the Ru−TiO_2 electron-tunneling distance being very similar for x = 0, 1, and 2. For all of the Rux sensitizers, a relatively small potential was needed for generation of current in the dark, indicating that the reaction between electrons in TiO_2 and the I_3^-/I^- electrolyte solution is as favorable for the Rux sensitizers as for unmodified TiO_2 electrodes.


Item Type:Article
Related URLs:
URLURL TypeDescription
http://dx.doi.org/10.1021/jp021921uDOIArticle
http://pubs.acs.org/doi/abs/10.1021/jp021921uPublisherArticle
ORCID:
AuthorORCID
Kuciauskas, Darius0000-0001-8091-5718
Lewis, Nathan S.0000-0001-5245-0538
Winkler, Jay R.0000-0002-4453-9716
Gray, Harry B.0000-0002-7937-7876
Additional Information:© 2003 American Chemical Society. Received 21 August 2002. Published online 11 April 2003. Published in print 1 May 2003. K.K. thanks the Carlsberg Foundation, Denmark, for a postdoctoral fellowship, and R.V. acknowledges the Link Foundation for funding. This work is supported through NREL subcontract (ACQ-1-30619-09) under DOE contract (DE-AC36-99-G010337). Work on the synthesis and characterization of the Rux complexes was supported by the NSF (H.B.G. and J.R.W.) and by the Arnold and Mabel Beckman Foundation.
Funders:
Funding AgencyGrant Number
Carlsberg FoundationUNSPECIFIED
Link FoundationUNSPECIFIED
National Renewable Energy LaboratoryACQ-1-30619-09
Department of Energy (DOE)DE-AC36-99-G010337
NSFUNSPECIFIED
Arnold and Mabel Beckman FoundationUNSPECIFIED
Issue or Number:18
DOI:10.1021/jp021921u
Record Number:CaltechAUTHORS:20170519-142727736
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20170519-142727736
Official Citation:Effects of Bridging Ligands on the Current−Potential Behavior and Interfacial Kinetics of Ruthenium-Sensitized Nanocrystalline TiO2 Photoelectrodes Kristine Kilså, Elizabeth I. Mayo, Darius Kuciauskas, Randy Villahermosa, Nathan S. Lewis, Jay R. Winkler, and Harry B. Gray The Journal of Physical Chemistry A 2003 107 (18), 3379-3383 DOI: 10.1021/jp021921u
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:77609
Collection:CaltechAUTHORS
Deposited By: Ruth Sustaita
Deposited On:22 May 2017 16:09
Last Modified:15 Nov 2021 17:32

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