H 2 -Evolving Dye-Sensitized Photocathode Based on a Ruthenium Diacetylide/Cobaloxime Supramolecular Assembly
Résumé
The development of NiO-based molecular photocathodes is attracting growing interest in the
field of dye-sensitized photoelectrochemical cells (DS-PEC) for efficient conversion of sunlight
into fuel. For this purpose different strategies are developed to assemble the molecular
components together in order to build functional devices. Here, an original dye-catalyst
supramolecular assembly was designed and obtained via axial coordination of a cobalt-based
H2-evolving catalyst, i.e. a cobaloxime complex, to a pyridyl-functionalized rutheniumdiacetylide photosensitizer. The new supramolecular assembly was successfully employed for
the construction of efficient NiO-based photocathodes for solar hydrogen production. We report
a joint experimental and theoretical study of the new photocatalytic system, including
electrochemical and XPS analyses. Photo-electrochemical generation of H2 under pertinent
aqueous conditions eventually led to a faradaic efficiency of 27 %
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