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Title: Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis

Abstract

Water oxidation is a critical step in artificial photosynthesis and provides the protons and electrons used in reduction reactions to make solar fuels. Significant advances have been made in the area of molecular water oxidation catalysts with a notable breakthrough in the development of Ru(II) complexes that use a planar “bda” ligand (bda is 2,2'-bipyridine-6,6'-dicarboxylate). These Ru(II)(bda) complexes show lower overpotentials for driving water oxidation making them ideal for light-driven applications with a suitable chromophore. Nevertheless, synthesis of heterogeneous Ru(II)(bda) complexes remains challenging. We discuss here a new “bottom-up” synthetic method for immobilizing these catalysts at the surface of a photoanode for use in a dye-sensitized photoelectrosynthesis cell (DSPEC). The procedure provides a basis for rapidly screening the role of ligand variations at the catalyst in order to understand the impact on device performance. The best results of a water-oxidation DSPEC photoanode based on this procedure reached 1.4 mA/cm 2 at pH 7 in 0.1 M [PO 4H 2]-/[PO 4H] 2- solution with minimal loss in catalytic behavior over 30 min, and produced an incident photon to current efficiency (IPCE) of 24.8% at 440 nm.

Authors:
 [1];  [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
  2. Florida Intl Univ., Miami, FL (United States). Dept. of Chemistry and Biochemistry
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) (SC-22)
OSTI Identifier:
1470086
Grant/Contract Number:  
SC0001011
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 2; 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 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
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

Wang, Degao, Marquard, Seth L., Troian-Gautier, Ludovic, Sheridan, Matthew V., Sherman, Benjamin D., Wang, Ying, Eberhart, Michael S., Farnum, Byron H., Dares, Christopher J., and Meyer, Thomas J. Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis. United States: N. p., 2018. Web. doi:10.1021/jacs.7b10809.
Wang, Degao, Marquard, Seth L., Troian-Gautier, Ludovic, Sheridan, Matthew V., Sherman, Benjamin D., Wang, Ying, Eberhart, Michael S., Farnum, Byron H., Dares, Christopher J., & Meyer, Thomas J. Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis. United States. doi:10.1021/jacs.7b10809.
Wang, Degao, Marquard, Seth L., Troian-Gautier, Ludovic, Sheridan, Matthew V., Sherman, Benjamin D., Wang, Ying, Eberhart, Michael S., Farnum, Byron H., Dares, Christopher J., and Meyer, Thomas J. Tue . "Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis". United States. doi:10.1021/jacs.7b10809. https://www.osti.gov/servlets/purl/1470086.
@article{osti_1470086,
title = {Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis},
author = {Wang, Degao and Marquard, Seth L. and Troian-Gautier, Ludovic and Sheridan, Matthew V. and Sherman, Benjamin D. and Wang, Ying and Eberhart, Michael S. and Farnum, Byron H. and Dares, Christopher J. and Meyer, Thomas J.},
abstractNote = {Water oxidation is a critical step in artificial photosynthesis and provides the protons and electrons used in reduction reactions to make solar fuels. Significant advances have been made in the area of molecular water oxidation catalysts with a notable breakthrough in the development of Ru(II) complexes that use a planar “bda” ligand (bda is 2,2'-bipyridine-6,6'-dicarboxylate). These Ru(II)(bda) complexes show lower overpotentials for driving water oxidation making them ideal for light-driven applications with a suitable chromophore. Nevertheless, synthesis of heterogeneous Ru(II)(bda) complexes remains challenging. We discuss here a new “bottom-up” synthetic method for immobilizing these catalysts at the surface of a photoanode for use in a dye-sensitized photoelectrosynthesis cell (DSPEC). The procedure provides a basis for rapidly screening the role of ligand variations at the catalyst in order to understand the impact on device performance. The best results of a water-oxidation DSPEC photoanode based on this procedure reached 1.4 mA/cm2 at pH 7 in 0.1 M [PO4H2]-/[PO4H]2- solution with minimal loss in catalytic behavior over 30 min, and produced an incident photon to current efficiency (IPCE) of 24.8% at 440 nm.},
doi = {10.1021/jacs.7b10809},
journal = {Journal of the American Chemical Society},
issn = {0002-7863},
number = 2,
volume = 140,
place = {United States},
year = {2018},
month = {1}
}

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