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Title: Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly

Abstract

The preparation and characterization of new Ru(II) polypyridyl-based chromophore–catalyst assemblies, [(4,4'-PO 3H 2-bpy) 2Ru(4-Mebpy-4'-epic)Ru(bda)(pic)] 2+ (1, bpy = 2,2'-bipyridine; 4-Mebpy-4'-epic = 4-(4-methylbipyridin-4'-yl-ethyl)-pyridine; bda = 2,2'-bipyridine-6,6'-dicarboxylate; pic = 4-picoline), and [(bpy) 2Ru(4-Mebpy-4'-epic)Ru(bda)(pic)] 2+ (1') are described, as is the application of 1 in a dye-sensitized photoelectrosynthesis cell (DSPEC) for solar water splitting. Furthermore, on SnO 2/TiO 2 core–shell electrodes in a DSPEC configuration with a Pt cathode, the chromophore–catalyst assembly undergoes light-driven water oxidation at pH 5.7 in a 0.1 M acetate buffer, 0.5 M in NaClO 4. We observed photocurrents of ~0.85 mA cm –2, with illumination by a 100 mW cm –2 white light source, after 30 s under a 0.1 V vs Ag/AgCl applied bias with a faradaic efficiency for O 2 production of 74% measured over a 5 min illumination period.

Authors:
ORCiD logo [1];  [2];  [1];  [1]; ORCiD logo [2];  [1];  [2]
  1. Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
Publication Date:
Research Org.:
Brookhaven National Lab. (BNL), Upton, NY (United States); 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:
1349575
Report Number(s):
BNL-113712-2017-JA
Journal ID: ISSN 2380-8195; R&D Project: CO026; KC0304030
Grant/Contract Number:  
SC0012704; SC0001011
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
ACS Energy Letters
Additional Journal Information:
Journal Volume: 2; Journal Issue: 1; Journal ID: ISSN 2380-8195
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Sherman, Benjamin D., Xie, Yan, Sheridan, Matthew V., Wang, Degao, Shaffer, David W., Meyer, Thomas J., and Concepcion, Javier J. Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly. United States: N. p., 2016. Web. doi:10.1021/acsenergylett.6b00661.
Sherman, Benjamin D., Xie, Yan, Sheridan, Matthew V., Wang, Degao, Shaffer, David W., Meyer, Thomas J., & Concepcion, Javier J. Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly. United States. https://doi.org/10.1021/acsenergylett.6b00661
Sherman, Benjamin D., Xie, Yan, Sheridan, Matthew V., Wang, Degao, Shaffer, David W., Meyer, Thomas J., and Concepcion, Javier J. Fri . "Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly". United States. https://doi.org/10.1021/acsenergylett.6b00661. https://www.osti.gov/servlets/purl/1349575.
@article{osti_1349575,
title = {Light-Driven Water Splitting by a Covalently Linked Ruthenium-Based Chromophore–Catalyst Assembly},
author = {Sherman, Benjamin D. and Xie, Yan and Sheridan, Matthew V. and Wang, Degao and Shaffer, David W. and Meyer, Thomas J. and Concepcion, Javier J.},
abstractNote = {The preparation and characterization of new Ru(II) polypyridyl-based chromophore–catalyst assemblies, [(4,4'-PO3H2-bpy)2Ru(4-Mebpy-4'-epic)Ru(bda)(pic)]2+ (1, bpy = 2,2'-bipyridine; 4-Mebpy-4'-epic = 4-(4-methylbipyridin-4'-yl-ethyl)-pyridine; bda = 2,2'-bipyridine-6,6'-dicarboxylate; pic = 4-picoline), and [(bpy)2Ru(4-Mebpy-4'-epic)Ru(bda)(pic)]2+ (1') are described, as is the application of 1 in a dye-sensitized photoelectrosynthesis cell (DSPEC) for solar water splitting. Furthermore, on SnO2/TiO2 core–shell electrodes in a DSPEC configuration with a Pt cathode, the chromophore–catalyst assembly undergoes light-driven water oxidation at pH 5.7 in a 0.1 M acetate buffer, 0.5 M in NaClO4. We observed photocurrents of ~0.85 mA cm–2, with illumination by a 100 mW cm–2 white light source, after 30 s under a 0.1 V vs Ag/AgCl applied bias with a faradaic efficiency for O2 production of 74% measured over a 5 min illumination period.},
doi = {10.1021/acsenergylett.6b00661},
url = {https://www.osti.gov/biblio/1349575}, journal = {ACS Energy Letters},
issn = {2380-8195},
number = 1,
volume = 2,
place = {United States},
year = {2016},
month = {12}
}

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