Charge Recombination Dynamics in Sensitized SnO2/TiO2 Core/Shell Photoanodes
Abstract
Studies have been conducted to examine the mechanisms of charge recombination in dye-sensitized SnO2/TiO2 core/shell films. Nanostructured SnO2/TiO2 core/shell films varying in TiO2 shell thicknesses were prepared via atomic layer deposition and sensitized with a phosphonate-derivatized ruthenium chromophore [Ru(bpy)2(4,4$$'$$-(PO3H2)2bpy)]2+. Transient absorption spectroscopy was used to study the interfacial charge recombination dynamics for these core/shell materials. Charge recombination for sensitized, as-deposited SnO2/TiO2 core/shell systems is dominated by a tunneling mechanism for shell thicknesses between 0 and 3.2 nm, with $$β$$ = 0.25 Å–1. For shell thicknesses greater than 3.2 nm, recombination primarily proceeds directly via electrons localized in the relatively thick TiO2 shell. Annealing the SnO2/TiO2 core/shell structure at 450°C affects the recombination dynamics substantially; charge recombination dynamics for the annealed films do not show a dependence on shell thickness and are comparable to ZrO2/TiO2 control samples, suggesting the annealing process perturbs the core/shell interface. This analysis of charge recombination dynamics indicates that there is an optimum shell thickness to maximize charge separation lifetimes in dye-sensitized core/shell photoanodes and that the nature of the core/shell interface influences the efficacy of these materials.
- Authors:
-
- Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1387237
- Grant/Contract Number:
- SC0001011
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 119; Journal Issue: 51; Related Information: UNC partners with University of North Carolina (lead); Duke University; University of Florida; Georgia Institute of Technology; University; North Carolina Central University; Research Triangle Institute; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis (homogeneous); catalysis (heterogeneous); solar (photovoltaic); solar (fuels); photosynthesis (natural and artificial); hydrogen and fuel cells; electrodes - solar; charge transport; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly)
Citation Formats
Knauf, Robin R., Kalanyan, Berç, Parsons, Gregory N., and Dempsey, Jillian L. Charge Recombination Dynamics in Sensitized SnO2/TiO2 Core/Shell Photoanodes. United States: N. p., 2015.
Web. doi:10.1021/acs.jpcc.5b10574.
Knauf, Robin R., Kalanyan, Berç, Parsons, Gregory N., & Dempsey, Jillian L. Charge Recombination Dynamics in Sensitized SnO2/TiO2 Core/Shell Photoanodes. United States. https://doi.org/10.1021/acs.jpcc.5b10574
Knauf, Robin R., Kalanyan, Berç, Parsons, Gregory N., and Dempsey, Jillian L. Thu .
"Charge Recombination Dynamics in Sensitized SnO2/TiO2 Core/Shell Photoanodes". United States. https://doi.org/10.1021/acs.jpcc.5b10574. https://www.osti.gov/servlets/purl/1387237.
@article{osti_1387237,
title = {Charge Recombination Dynamics in Sensitized SnO2/TiO2 Core/Shell Photoanodes},
author = {Knauf, Robin R. and Kalanyan, Berç and Parsons, Gregory N. and Dempsey, Jillian L.},
abstractNote = {Studies have been conducted to examine the mechanisms of charge recombination in dye-sensitized SnO2/TiO2 core/shell films. Nanostructured SnO2/TiO2 core/shell films varying in TiO2 shell thicknesses were prepared via atomic layer deposition and sensitized with a phosphonate-derivatized ruthenium chromophore [Ru(bpy)2(4,4$'$-(PO3H2)2bpy)]2+. Transient absorption spectroscopy was used to study the interfacial charge recombination dynamics for these core/shell materials. Charge recombination for sensitized, as-deposited SnO2/TiO2 core/shell systems is dominated by a tunneling mechanism for shell thicknesses between 0 and 3.2 nm, with $β$ = 0.25 Å–1. For shell thicknesses greater than 3.2 nm, recombination primarily proceeds directly via electrons localized in the relatively thick TiO2 shell. Annealing the SnO2/TiO2 core/shell structure at 450°C affects the recombination dynamics substantially; charge recombination dynamics for the annealed films do not show a dependence on shell thickness and are comparable to ZrO2/TiO2 control samples, suggesting the annealing process perturbs the core/shell interface. This analysis of charge recombination dynamics indicates that there is an optimum shell thickness to maximize charge separation lifetimes in dye-sensitized core/shell photoanodes and that the nature of the core/shell interface influences the efficacy of these materials.},
doi = {10.1021/acs.jpcc.5b10574},
journal = {Journal of Physical Chemistry. C},
number = 51,
volume = 119,
place = {United States},
year = {Thu Dec 10 00:00:00 EST 2015},
month = {Thu Dec 10 00:00:00 EST 2015}
}
Web of Science
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