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1.
Chemphyschem ; 18(22): 3274-3279, 2017 Nov 17.
Artículo en Inglés | MEDLINE | ID: mdl-28985010

RESUMEN

Multiple approaches will be needed to reduce the atmospheric CO2 levels, which have been linked to the undesirable effects of global climate change. The electroreduction of CO2 driven by renewable energy is one approach to reduce CO2 emissions while producing chemical building blocks, but current electrocatalysts exhibit low activity and selectivity. Here, we report the structural and electrochemical characterization of a promising catalyst for the electroreduction of CO2 to CO: Au nanoparticles supported on polymer-wrapped multiwall carbon nanotubes. This catalyst exhibits high selectivity for CO over H2 : 80-92 % CO, as well as high activity: partial current density for CO as high as 160 mA cm-2 . The observed high activity, originating from a high electrochemically active surface area (23 m2 g-1 Au), in combination with the low loading (0.17 mg cm-2 ) of the highly dispersed Au nanoparticles underscores the promise of this catalyst for efficient electroreduction of CO2 .

2.
J Am Chem Soc ; 134(48): 19520-3, 2012 Dec 05.
Artículo en Inglés | MEDLINE | ID: mdl-23167268

RESUMEN

The synthesis and application of carbon-supported, nitrogen-based organometallic silver catalysts for the reduction of CO(2) is studied using an electrochemical flow reactor. Their performance toward the selective formation of CO is similar to the performance achieved when using Ag as the catalyst, but comparatively at much lower silver loading. Faradaic efficiencies of the organometallic catalyst are higher than 90%, which are comparable to those of Ag. Furthermore, with the addition of an amine ligand to Ag/C, the partial current density for CO increases significantly, suggesting a possible co-catalyst mechanism. Additional improvements in activity and selectivity may be achieved as greater insight is obtained on the mechanism of CO(2) reduction and on how these complexes assemble on the carbon support.

3.
ChemSusChem ; 10(6): 1094-1099, 2017 03 22.
Artículo en Inglés | MEDLINE | ID: mdl-27791338

RESUMEN

We report characterization of a non-precious metal-free catalyst for the electrochemical reduction of CO2 to CO; namely, a pyrolyzed carbon nitride and multiwall carbon nanotube composite. This catalyst exhibits a high selectivity for production of CO over H2 (approximately 98 % CO and 2 % H2 ), as well as high activity in an electrochemical flow cell. The CO partial current density at intermediate cathode potentials (V=-1.46 V vs. Ag/AgCl) is up to 3.5× higher than state-of-the-art Ag nanoparticle-based catalysts, and the maximum current density is 90 mA cm-2 . The mass activity and energy efficiency (up to 48 %) were also higher than the Ag nanoparticle reference. Moving away from precious metal catalysts without sacrificing activity or selectivity may significantly enhance the prospects of electrochemical CO2 reduction as an approach to reduce atmospheric CO2 emissions or as a method for load-leveling in relation to the use of intermittent renewable energy sources.


Asunto(s)
Dióxido de Carbono/química , Monóxido de Carbono/química , Carbono/química , Conductividad Eléctrica , Nanotubos de Carbono/química , Nitrógeno/química , Catálisis , Electroquímica , Electrodos , Modelos Moleculares , Conformación Molecular , Nanocompuestos/química , Nitrilos/química , Oxidación-Reducción
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