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L3.03 - Atomic-Level Insights on Elevated-Temperature CO Oxidation and CO Reduction on Ceria-Based Electrocatalysts Revealed through In-Operando X-Ray Spectroscopy 
Date/Time:
April 22, 2014   4:15pm - 4:30pm
 
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The efficient electro-reduction of CO to chemical fuel, and the electro-oxidation of hydrocarbons are critical towards a carbon-neutral energy cycle. The simplest reactions involving carbon species in solid-oxide fuel cells and electrolyzer cells are CO oxidation and CO reduction, respectively. In catalyzing these reactions, doped ceria has been employed as a robust and highly active electrocatalyst. However, many controversies still remain about the reaction intermediates and the rate-determining step, despite numerous theoretical and experimental investigations.We employed synchrotron-based ambient pressure X-ray photoelectron spectroscopy and electrochemical impedance spectroscopy to investigate CO/CO electrochemical reactions on ceria under technologically-relevant conditions. By exposing ceria thin film in 300 mTorr of CO at various temperatures, we confirmed that carbonates are the primary adsorbate. Furthermore, using a microfabricated electrochemical cell, we applied various anodic and cathodic voltages to drive the reactions away from equilibrium at elevated temperature. We followed the changes in oxygen, carbon and Ce species under anodic and cathodic biases. In this talk, we will provide a new perspective on the electrochemical CO/CO conversion pathway on the surface of ceria.
 


 
 
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