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Title: Layer-by-Layer Molecular Assemblies for Dye-Sensitized Photoelectrosynthesis Cells Prepared by Atomic Layer Deposition

Abstract

In a Dye Sensitized Photoelectrosynthesis Cell (DSPEC) the relative orientation of catalyst and chromophore play important roles. Here we introduce a new, robust, Atomic Layer Deposition (ALD) procedure for the preparation of assemblies on wide bandgap semiconductors. In the procedure, phosphonated metal complex precursors react with metal ion bridging to an external chromophore or catalyst to give assemblies bridged by Al(III), Sn(IV), Ti(IV), or Zr(IV) metal oxide units as bridges. The procedure has been extended to chromophore-catalyst assemblies for water oxidation catalysis. A SnO2 bridged assembly on SnO2/TiO2 core/shell electrodes undergoes water splitting with an incident photon conversion efficiency (IPCE) of 17.1% at 440 nm. Reduction of water at a Ni(II)-based catalyst on NiO films has been shown to give H2. Compared to conventional solution-based procedures, the ALD approach offers significant advantages in scope and flexibility for the preparation of stable surface structures.

Authors:
 [1];  [1];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [2];  [3]; ORCiD logo [3]; ORCiD logo [1]
  1. Department of Chemistry, University of North Carolina at Chapel Hill, Chapel Hill, North Carolina 27599, United States
  2. Department of Chemistry and Biochemistry, Florida International University, 11200 SW 8th St, Miami, Florida 33199, United States
  3. Center for Molecular Electrocatalysis, Physical Sciences Division, Pacific Northwest National Laboratory, P.O. Box 999, K2-12, Richland, Washington 99352, United States
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1406772
Report Number(s):
PNNL-SA-125900
Journal ID: ISSN 0002-7863; KC0307010
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of the American Chemical Society; Journal Volume: 139; Journal Issue: 41
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; DSPEC; core/shell; Atomic Layer Deposition; self-assemble; water splitting

Citation Formats

Wang, Degao, Sheridan, Matthew V., Shan, Bing, Farnum, Byron H., Marquard, Seth L., Sherman, Benjamin D., Eberhart, Michael S., Nayak, Animesh, Dares, Christopher J., Das, Atanu K., Bullock, R. Morris, and Meyer, Thomas J. Layer-by-Layer Molecular Assemblies for Dye-Sensitized Photoelectrosynthesis Cells Prepared by Atomic Layer Deposition. United States: N. p., 2017. Web. doi:10.1021/jacs.7b07216.
Wang, Degao, Sheridan, Matthew V., Shan, Bing, Farnum, Byron H., Marquard, Seth L., Sherman, Benjamin D., Eberhart, Michael S., Nayak, Animesh, Dares, Christopher J., Das, Atanu K., Bullock, R. Morris, & Meyer, Thomas J. Layer-by-Layer Molecular Assemblies for Dye-Sensitized Photoelectrosynthesis Cells Prepared by Atomic Layer Deposition. United States. doi:10.1021/jacs.7b07216.
Wang, Degao, Sheridan, Matthew V., Shan, Bing, Farnum, Byron H., Marquard, Seth L., Sherman, Benjamin D., Eberhart, Michael S., Nayak, Animesh, Dares, Christopher J., Das, Atanu K., Bullock, R. Morris, and Meyer, Thomas J. Wed . "Layer-by-Layer Molecular Assemblies for Dye-Sensitized Photoelectrosynthesis Cells Prepared by Atomic Layer Deposition". United States. doi:10.1021/jacs.7b07216.
@article{osti_1406772,
title = {Layer-by-Layer Molecular Assemblies for Dye-Sensitized Photoelectrosynthesis Cells Prepared by Atomic Layer Deposition},
author = {Wang, Degao and Sheridan, Matthew V. and Shan, Bing and Farnum, Byron H. and Marquard, Seth L. and Sherman, Benjamin D. and Eberhart, Michael S. and Nayak, Animesh and Dares, Christopher J. and Das, Atanu K. and Bullock, R. Morris and Meyer, Thomas J.},
abstractNote = {In a Dye Sensitized Photoelectrosynthesis Cell (DSPEC) the relative orientation of catalyst and chromophore play important roles. Here we introduce a new, robust, Atomic Layer Deposition (ALD) procedure for the preparation of assemblies on wide bandgap semiconductors. In the procedure, phosphonated metal complex precursors react with metal ion bridging to an external chromophore or catalyst to give assemblies bridged by Al(III), Sn(IV), Ti(IV), or Zr(IV) metal oxide units as bridges. The procedure has been extended to chromophore-catalyst assemblies for water oxidation catalysis. A SnO2 bridged assembly on SnO2/TiO2 core/shell electrodes undergoes water splitting with an incident photon conversion efficiency (IPCE) of 17.1% at 440 nm. Reduction of water at a Ni(II)-based catalyst on NiO films has been shown to give H2. Compared to conventional solution-based procedures, the ALD approach offers significant advantages in scope and flexibility for the preparation of stable surface structures.},
doi = {10.1021/jacs.7b07216},
journal = {Journal of the American Chemical Society},
number = 41,
volume = 139,
place = {United States},
year = {Wed Aug 30 00:00:00 EDT 2017},
month = {Wed Aug 30 00:00:00 EDT 2017}
}