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

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:
Report Number(s):
BNL-113712-2017-JA
Journal ID: ISSN 2380-8195; R&D Project: CO026; KC0304030
Grant/Contract Number:
SC00112704; SC0001011
Type:
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)
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1349575