Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 135, Issue 32, Pages 11861-11868Publisher
AMER CHEMICAL SOC
DOI: 10.1021/ja404158r
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Funding
- Office of Science of the U.S. Department of Energy [DE-SC0004993]
- [DE-AC02-05CH11231]
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Molecular cobalt-containing hydrogen production catalysts are grafted to a visible-light-absorbing semiconductor. The attachment procedure exploits the UV-induced immobilization chemistry of vinylpyridine to p-type (100) gallium phosphide (GaP). Single step surface-initiated photopolymerization yields a covalently attached polymer with pendent pyridyl groups that provide attachment points for assembling cobaloxime catalysts. Successful attachment is characterized by grazing angle attenuated total reflection Fourier transform infrared spectroscopy (GATR-FTIR), which shows distinct vibrational modes associated with the catalyst, as well as X-ray photoelectron spectroscopy (XPS) and X-ray absorption near edge structure spectroscopy (XANES) that confirm the presence of intact Co-III complex on the surface. The Co-functionalized photocathode shows significantly enhanced photoelectrochemical (PEC) performance in aqueous conditions at neutral pH, compared to results obtained on GaP without attached cobalt complex PEC measurements, at 100 mW cm(-2) illumination, yield a 2.4 mA cm(-2) current density at a 310 mV underpotential.
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