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

Sherman, Benjamin D.; Xie, Yan; Sheridan, Matthew V.; Wang, Degao; Shaffer, David W.; Meyer, Thomas J.; Concepcion, Javier J.

doi:10.1021/acsenergylett.6b00661

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

Journal Article · Thu Dec 08 23:00:00 EST 2016 · ACS Energy Letters

DOI:https://doi.org/10.1021/acsenergylett.6b00661· OSTI ID:1349575

^[1]; Xie, Yan ^[2]; Sheridan, Matthew V. ^[1]; Wang, Degao ^[1]; ^[2]; Meyer, Thomas J. ^[1]; Concepcion, Javier J. ^[2]

Univ. of North Carolina, Chapel Hill, NC (United States). Dept. of Chemistry
Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division

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.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: SC0012704; SC0001011

OSTI ID:: 1349575

Report Number(s):: BNL--113712-2017-JA; KC0304030

Journal Information:: ACS Energy Letters, Journal Name: ACS Energy Letters Journal Issue: 1 Vol. 2; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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