Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis.

Autor: Wang D; Department of Chemistry, University of North Carolina Chapel Hill , Chapel Hill, North Carolina 27599, United States., Marquard SL; Department of Chemistry, University of North Carolina Chapel Hill , Chapel Hill, North Carolina 27599, United States., Troian-Gautier L; Department of Chemistry, University of North Carolina Chapel Hill , Chapel Hill, North Carolina 27599, United States., Sheridan MV; Department of Chemistry, University of North Carolina Chapel Hill , Chapel Hill, North Carolina 27599, United States., Sherman BD; Department of Chemistry, University of North Carolina Chapel Hill , Chapel Hill, North Carolina 27599, United States., Wang Y; Department of Chemistry, University of North Carolina Chapel Hill , Chapel Hill, North Carolina 27599, United States., Eberhart MS; Department of Chemistry, University of North Carolina Chapel Hill , Chapel Hill, North Carolina 27599, United States., Farnum BH; Department of Chemistry, University of North Carolina Chapel Hill , Chapel Hill, North Carolina 27599, United States., Dares CJ; Department of Chemistry and Biochemistry, Florida International University , 11200 SW Eighth Street, Miami, Florida 33199, United States., Meyer TJ; Department of Chemistry, University of North Carolina Chapel Hill , Chapel Hill, North Carolina 27599, United States.
Jazyk: angličtina
Zdroj: Journal of the American Chemical Society [J Am Chem Soc] 2018 Jan 17; Vol. 140 (2), pp. 719-726. Date of Electronic Publication: 2018 Jan 02.
DOI: 10.1021/jacs.7b10809
Abstrakt: Water oxidation is a critical step in artificial photosynthesis and provides the protons and electrons used in reduction reactions to make solar fuels. Significant advances have been made in the area of molecular water oxidation catalysts with a notable breakthrough in the development of Ru(II) complexes that use a planar "bda" ligand (bda is 2,2'-bipyridine-6,6'-dicarboxylate). These Ru(II)(bda) complexes show lower overpotentials for driving water oxidation making them ideal for light-driven applications with a suitable chromophore. Nevertheless, synthesis of heterogeneous Ru(II)(bda) complexes remains challenging. We discuss here a new "bottom-up" synthetic method for immobilizing these catalysts at the surface of a photoanode for use in a dye-sensitized photoelectrosynthesis cell (DSPEC). The procedure provides a basis for rapidly screening the role of ligand variations at the catalyst in order to understand the impact on device performance. The best results of a water-oxidation DSPEC photoanode based on this procedure reached 1.4 mA/cm 2 at pH 7 in 0.1 M [PO 4 H 2 ] - /[PO 4 H] 2- solution with minimal loss in catalytic behavior over 30 min, and produced an incident photon to current efficiency (IPCE) of 24.8% at 440 nm.
Databáze: MEDLINE
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