Efficient Light-Driven Oxidation of Alcohols Using an Organic Chromophore–Catalyst Assembly Anchored to TiO2

Pho, Toan V.; Sheridan, Matthew V.; Morseth, Zachary A.; Sherman, Benjamin D.; Meyer, Thomas J.; Papanikolas, John M.; Schanze, Kirk S.; Reynolds, John R.

doi:10.1021/acsami.6b00932

Title: Efficient Light-Driven Oxidation of Alcohols Using an Organic Chromophore–Catalyst Assembly Anchored to TiO₂

Journal Article · Thu Mar 31 00:00:00 EDT 2016 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.6b00932· OSTI ID:1371253

Pho, Toan V. ^[1]; Sheridan, Matthew V. ^[2]; Morseth, Zachary A. ^[2]; Sherman, Benjamin D. ^[2]; Meyer, Thomas J. ^[2]; Papanikolas, John M. ^[2]; Schanze, Kirk S. ^[3]; Reynolds, John R. ^[1]

Georgia Inst. of Technology, Atlanta, GA (United States)
Univ. of North Carolina, Chapel Hill, NC (United States)
Univ. of Florida, Gainesville, FL (United States)

In this work, the ligand 5-PO₃H₂-2,2':5',2"-terthiophene-5-trpy, T3 (trpy = 2,2':6',2"-terpyridine), was prepared and studied in aqueous solutions along with its metal complex assembly [Ru(T3)(bpy)(OH₂)]²⁺ (T3-Ru-OH₂, bpy = 2,2'-bipyridine). T3 contains a phosphonic acid group for anchoring to a TiO₂ photoanode under aqueous conditions, a terthiophene fragment for light absorption and electron injection into TiO₂, and a terminal trpy ligand for the construction of assemblies comprising a molecular oxidation catalyst. At a TiO₂ photoanode, T3 displays efficient injection at pH 4.35 as evidenced by the high photocurrents (~350 uA/cm²) arising from hydroquinone oxidation. Addition of [Ru(bpy)(OTf)][OTf]₂ (bpy = 2,2'-bipyridine, OTf^– = triflate) to T3 at the free trpy ligand forms the molecular assembly, T3-Ru-OH₂, with the oxidative catalyst fragment: [Ru(trpy)(bpy)(OH₂)]²⁺. Finally, the new assembly, T3-Ru-OH₂, was used to perform efficient light-driven oxidation of phenol (230 μA/cm²) and benzyl alcohol (25 μA/cm²) in a dye-sensitized photoelectrosynthesis cell.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Solar Fuels (UNC EFRC)

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

Grant/Contract Number:: SC0001011

OSTI ID:: 1371253

Journal Information:: ACS Applied Materials and Interfaces, Vol. 8, Issue 14; 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; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 32 works

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
C−H activation
organic alcohol oxidation
dye-sensitized solar cell
dye-sensitized photoelectrosynthesis cell
solar fuels

Title: Efficient Light-Driven Oxidation of Alcohols Using an Organic Chromophore–Catalyst Assembly Anchored to TiO2

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Title: Efficient Light-Driven Oxidation of Alcohols Using an Organic Chromophore–Catalyst Assembly Anchored to TiO₂