Potential-Dependent Adsorption of CO and Its Low-Overpotential Reduction to CH3CH2OH on Cu(511) Surface Reconstructed from Cu(pc): Operando Studies by Seriatim STM-EQCN-DEMS (original) (raw)

Tracking a Common Surface-Bound Intermediate during CO2-to-Fuels Catalysis

ACS central science, 2016

Rational design of selective CO2-to-fuels electrocatalysts requires direct knowledge of the electrode surface structure during turnover. Metallic Cu is the most versatile CO2-to-fuels catalyst, capable of generating a wide array of value-added products, including methane, ethylene, and ethanol. All of these products are postulated to form via a common surface-bound CO intermediate. Therefore, the kinetics and thermodynamics of CO adsorption to Cu play a central role in determining fuel-formation selectivity and efficiency, highlighting the need for direct observation of CO surface binding equilibria under catalytic conditions. Here, we synthesize nanostructured Cu films adhered to IR-transparent Si prisms, and we find that these Cu surfaces enhance IR absorption of bound molecules. Using these films as electrodes, we examine Cu-catalyzed CO2 reduction in situ via IR spectroelectrochemistry. We observe that Cu surfaces bind electrogenerated CO, derived from CO2, beginning at -0.60 V ...

CO2 activation over catalytic surfaces

Chemphyschem : a European journal of chemical physics and physical chemistry, 2017

This article describes the main strategies to activate and convert carbon dioxide (CO2) into valuable chemicals over catalytic surfaces. Coherent elements such as common intermediates are identified in the different strategies and concisely discussed based on the reactivity of CO2 with the aim to understand the decisive factors for selective and efficient CO2 conversion.