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Title: Linker Length-Dependent Electron-Injection Dynamics of Trimesitylporphyrins on SnO 2 Films

Abstract

Electron-injection dynamics of dye-sensitized photoelectrochemical cells depend on the length of the linker connecting the molecular photosensitizer to the metal oxide electron acceptor. However, systematic studies of the effect of chromophore–oxide distance are scarce. In this work, we present the synthesis, characterization, spectroscopy, and computational modeling of electron-injection dynamics from free-base trimesitylporphyrins with varying linker lengths into tin(IV) oxide (SnO 2). In each system, the porphyrin core and metal oxide film remain the same while only the linker binding the porphyrin to the carboxylate anchor group is varied. A length range spanning 8.5–17.2 Å is studied by employing phenylene, biphenylene, terphenylene, and benzanilide groups as the linker. We find a clear correlation between linker length and injection rates, providing insights that will be exploited in the optimization of dye-sensitized photoelectrochemical cells.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Yale Univ., New Haven, CT (United States). Dept. of Chemistry, and Yale Energy Sciences Inst.
  2. Yale Univ., New Haven, CT (United States). Dept. of Chemistry, and Yale Energy Sciences Inst.; Stockholm Univ. (Sweden). Dept. of Physics
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1483383
Grant/Contract Number:  
[FG02-07ER15909]
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
[ Journal Volume: 121; Journal Issue: 41]; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; electron injection; trimesitylporphyrins; terahertz spectroscopy; density functional theory

Citation Formats

Lee, Shin Hee, Regan, Kevin P., Hedström, Svante, Matula, Adam J., Chaudhuri, Subhajyoti, Crabtree, Robert H., Batista, Victor S., Schmuttenmaer, Charles A., and Brudvig, Gary W. Linker Length-Dependent Electron-Injection Dynamics of Trimesitylporphyrins on SnO2 Films. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.7b07855.
Lee, Shin Hee, Regan, Kevin P., Hedström, Svante, Matula, Adam J., Chaudhuri, Subhajyoti, Crabtree, Robert H., Batista, Victor S., Schmuttenmaer, Charles A., & Brudvig, Gary W. Linker Length-Dependent Electron-Injection Dynamics of Trimesitylporphyrins on SnO2 Films. United States. doi:10.1021/acs.jpcc.7b07855.
Lee, Shin Hee, Regan, Kevin P., Hedström, Svante, Matula, Adam J., Chaudhuri, Subhajyoti, Crabtree, Robert H., Batista, Victor S., Schmuttenmaer, Charles A., and Brudvig, Gary W. Thu . "Linker Length-Dependent Electron-Injection Dynamics of Trimesitylporphyrins on SnO2 Films". United States. doi:10.1021/acs.jpcc.7b07855. https://www.osti.gov/servlets/purl/1483383.
@article{osti_1483383,
title = {Linker Length-Dependent Electron-Injection Dynamics of Trimesitylporphyrins on SnO2 Films},
author = {Lee, Shin Hee and Regan, Kevin P. and Hedström, Svante and Matula, Adam J. and Chaudhuri, Subhajyoti and Crabtree, Robert H. and Batista, Victor S. and Schmuttenmaer, Charles A. and Brudvig, Gary W.},
abstractNote = {Electron-injection dynamics of dye-sensitized photoelectrochemical cells depend on the length of the linker connecting the molecular photosensitizer to the metal oxide electron acceptor. However, systematic studies of the effect of chromophore–oxide distance are scarce. In this work, we present the synthesis, characterization, spectroscopy, and computational modeling of electron-injection dynamics from free-base trimesitylporphyrins with varying linker lengths into tin(IV) oxide (SnO2). In each system, the porphyrin core and metal oxide film remain the same while only the linker binding the porphyrin to the carboxylate anchor group is varied. A length range spanning 8.5–17.2 Å is studied by employing phenylene, biphenylene, terphenylene, and benzanilide groups as the linker. We find a clear correlation between linker length and injection rates, providing insights that will be exploited in the optimization of dye-sensitized photoelectrochemical cells.},
doi = {10.1021/acs.jpcc.7b07855},
journal = {Journal of Physical Chemistry. C},
number = [41],
volume = [121],
place = {United States},
year = {2017},
month = {9}
}

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Figures / Tables:

Figure 1 Figure 1: Molecular structures of trimesitylporphyrins used in this study.

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