TY - JOUR
T1 - Interfacial Deposition of Ru(II) Bipyridine-Dicarboxylate Complexes by Ligand Substitution for Applications in Water Oxidation Catalysis
AU - Wang, Degao
AU - Marquard, Seth L.
AU - Troian-Gautier, Ludovic
AU - Sheridan, Matthew V.
AU - Sherman, Benjamin D.
AU - Wang, Ying
AU - Eberhart, Michael S.
AU - Farnum, Byron H.
AU - Dares, Christopher J.
AU - Meyer, Thomas J.
N1 - Publisher Copyright:
© 2017 American Chemical Society.
PY - 2018/1/17
Y1 - 2018/1/17
N2 - 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/cm2 at pH 7 in 0.1 M [PO4H2]-/[PO4H]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.
AB - 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/cm2 at pH 7 in 0.1 M [PO4H2]-/[PO4H]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.
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U2 - 10.1021/jacs.7b10809
DO - 10.1021/jacs.7b10809
M3 - Article
C2 - 29232507
AN - SCOPUS:85040673556
SN - 0002-7863
VL - 140
SP - 719
EP - 726
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 2
ER -