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1.
Proc Natl Acad Sci U S A ; 113(20): 5526-9, 2016 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-27140621

RESUMO

Low-cost, efficient CO2-to-CO+O2 electrochemical splitting is a key step for liquid-fuel production for renewable energy storage and use of CO2 as a feedstock for chemicals. Heterogeneous catalysts for cathodic CO2-to-CO associated with an O2-evolving anodic reaction in high-energy-efficiency cells are not yet available. An iron porphyrin immobilized into a conductive Nafion/carbon powder layer is a stable cathode producing CO in pH neutral water with 90% faradaic efficiency. It is coupled with a water oxidation phosphate cobalt oxide anode in a home-made electrolyzer by means of a Nafion membrane. Current densities of approximately 1 mA/cm(2) over 30-h electrolysis are achieved at a 2.5-V cell voltage, splitting CO2 and H2O into CO and O2 with a 50% energy efficiency. Remarkably, CO2 reduction outweighs the concurrent water reduction. The setup does not prevent high-efficiency proton transport through the Nafion membrane separator: The ohmic drop loss is only 0.1 V and the pH remains stable. These results demonstrate the possibility to set up an efficient, low-voltage, electrochemical cell that converts CO2 into CO and O2 by associating a cathodic-supported molecular catalyst based on an abundant transition metal with a cheap, easy-to-prepare anodic catalyst oxidizing water into O2.

2.
Phys Chem Chem Phys ; 11(18): 3573-9, 2009 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-19421563

RESUMO

Carbon supported Au-Pt catalysts with different bimetallic compositions were prepared by water-in-oil (w/o) micro-emulsions. Carbon Vulcan XC-72R was added during the synthesis of particles in order to obtain good dispersion. Structural characterization was performed using XRD (X-ray diffraction) at wide angles, WAXS (wide-angle X-ray scattering) which showed that Pt-Au particles exhibited alloy properties in samples with high gold-content, and a segregation effect for those with low gold-content. Electrochemical characterization allowed estimation of the surface composition of Pt-Au alloys. These experiments have been confirmed by XRD data. Moreover, HRTEM (high resolution transmission electron microscopy) and XEDS (X-ray energy dispersive spectroscopy) characterization further confirmed the electrochemical results and XRD data. CO stripping experiments have shown an increasing bonding energy between CO and platinum with the gold content in the nanoalloys.

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