School of Chemistry & Biochemistry, School of Materials Science & Engineering, Center for Organic Photonics and Electronics, Georgia Tech Polymer Network, Georgia Institute of Technology , Atlanta, Georgia 30332, United States.
Department of Chemistry, University of North Carolina at Chapel Hill , Chapel Hill, North Carolina 27599, United States.
ACS Appl Mater Interfaces. 2016 Apr 13;8(14):9125-33. doi: 10.1021/acsami.6b00932. Epub 2016 Mar 31.
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) (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/cm(2)) 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). The new assembly, T3-Ru-OH2, was used to perform efficient light-driven oxidation of phenol (230 μA/cm(2)) and benzyl alcohol (25 μA/cm(2)) in a dye-sensitized photoelectrosynthesis cell.
配体 5-PO3H2-2,2':5',2″-三联噻吩-5-三吡啶，T3（trpy = 2,2':6',2″-三联吡啶），在水溶液中与金属配合物组装物Ru(T3)(bpy)(OH2)（T3-Ru-OH2，bpy = 2,2'-联吡啶）一起被制备和研究。T3 含有一个磷酸基团，用于在水相条件下锚定在 TiO2 光阳极上，一个三联噻吩片段用于光吸收和电子注入 TiO2，以及一个末端三吡啶配体用于构建包含分子氧化催化剂的组装体。在 TiO2 光阳极上，T3 在 pH 4.35 时表现出高效注入，这表现为对苯二酚氧化产生的高光电流（约 350 uA/cm2）。在 T3 的游离三吡啶配体处添加[Ru(bpy)(OTf)][OTf]2（bpy = 2,2'-联吡啶，OTf(-) = 三氟甲磺酸根），形成分子组装体 T3-Ru-OH2，其中含有氧化催化剂片段：Ru(trpy)(bpy)(OH2)。新组装体 T3-Ru-OH2 用于在染料敏化光电合成电池中高效地进行苯酚（230 μA/cm2）和苄醇（25 μA/cm2）的光驱动氧化。
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