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CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface

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TLDR
A copper electrocatalyst at an abrupt reaction interface in an alkaline electrolyte reduces CO2 to ethylene with 70% faradaic efficiency at a potential of −0.55 volts versus a reversible hydrogen electrode (RHE).
Abstract
Carbon dioxide (CO 2 ) electroreduction could provide a useful source of ethylene, but low conversion efficiency, low production rates, and low catalyst stability limit current systems. Here we report that a copper electrocatalyst at an abrupt reaction interface in an alkaline electrolyte reduces CO 2 to ethylene with 70% faradaic efficiency at a potential of −0.55 volts versus a reversible hydrogen electrode (RHE). Hydroxide ions on or near the copper surface lower the CO 2 reduction and carbon monoxide (CO)–CO coupling activation energy barriers; as a result, onset of ethylene evolution at −0.165 volts versus an RHE in 10 molar potassium hydroxide occurs almost simultaneously with CO production. Operational stability was enhanced via the introduction of a polymer-based gas diffusion layer that sandwiches the reaction interface between separate hydrophobic and conductive supports, providing constant ethylene selectivity for an initial 150 operating hours.

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Citations
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Journal ArticleDOI

Speciation of Cu Surfaces During the Electrochemical CO Reduction Reaction.

TL;DR: In-situ surface enhanced Raman spectroscopy is employed to investigate the speciation of four commonly used Cu surfaces, i.e., Cu foil, Cu micro/nanoparticles, electrochemically deposited Cu film and oxide-derived Cu, at potentials relevant to the CO reduction reaction in an alkaline electrolyte and concludes that the oxygen containing surface species are unlikely to be active in facilitating the formation of C2+ oxygenates in theCO reduction reaction.
Journal ArticleDOI

High-Rate CO2 Electroreduction to C2+ Products over a Copper-Copper Iodide Catalyst.

TL;DR: In this article, the authors designed a Cu-CuI composite catalyst with abundant Cu0 /Cu+ interfaces by physically mixing Cu nanoparticles and CuI powders, which achieved a remarkable C2+ partial current density of 591 mA cm-2 at -10 V vs reversible hydrogen electrode in a flow cell.
Journal ArticleDOI

Efficient Methane Electrosynthesis Enabled by Tuning Local CO2 Availability.

TL;DR: These findings offer routes to produce methane with high FE and high conversion rate in CO2RR, and also to make direct use of dilute CO2 feedstocks.
Journal ArticleDOI

Electroreduction of CO2 to Formate on a Copper-Based Electrocatalyst at High Pressures with High Energy Conversion Efficiency.

TL;DR: A novel Cu2O nanoparticle film is synthesized by square-wave (SW) electrochemical redox cycling of high purity Cu foils and found important to afford near ~100% CO2 reduction to formate, which has implications toCO2 reduction into a single liquid product with high energy conversion efficiency.
Journal ArticleDOI

Electrolyte Effects on the Electrochemical Reduction of CO2.

TL;DR: An overview of recently obtained insights on electrolyte effects on the electrochemical reduction of CO2 is provided and how these insights can be used as design parameters for the construction of new electrocatalytic systems are discussed.
References
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Journal ArticleDOI

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Journal ArticleDOI

Improved tangent estimate in the nudged elastic band method for finding minimum energy paths and saddle points

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Journal ArticleDOI

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