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Journal ArticleDOI

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

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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What would it take for renewably powered electrosynthesis to displace petrochemical processes

TL;DR: A comparative analysis of electrocatalyst and carbon emissions assessment of CO2 products such as ethylene, ethanol, and carbon monoxide shows that electrocatalytic production has the potential to yield the greatest reduction in carbon emissions, provided that a steady supply of clean electricity is available.
Journal ArticleDOI

Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels

TL;DR: In this article, the authors review recent advances and challenges in the understanding of electrochemical CO2 reduction and discuss existing models for the initial activation of CO2 on the electrocatalyst and their importance for understanding selectivity.
Journal ArticleDOI

Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products

TL;DR: In this article, the authors discuss strategies to achieve high selectivity towards multicarbon products via rational catalyst and electrolyte design, focusing on findings extracted from in situ and operando characterizations.
Journal ArticleDOI

CO2 electrolysis to multicarbon products at activities greater than 1 A cm−2

TL;DR: A catalyst:ionomer bulk heterojunction (CIBH) architecture that decouples gas, ion, and electron transport and achieves CO2 electroreduction on copper in 7 M potassium hydroxide electrolyte with an ethylene partial current density at 45% cathodic energy efficiency.
References
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Journal ArticleDOI

The Importance of Cannizzaro-Type Reactions during Electrocatalytic Reduction of Carbon Dioxide

TL;DR: A seemingly catalytically inactive electrode, boron-doped diamond (BDD), is found to be active for CO2 and CO reduction to formaldehyde and even methane, and the results obtained here may explain the concomitant formation of acids and alcohols often observed during CO2 reduction.
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Nanomorphology-Enhanced Gas-Evolution Intensifies CO2 Reduction Electrochemistry

TL;DR: In this article, the morphology of nanostructured electrodes enhances long-range CO2 transport via their influence on gas-evolution, leading to a 4-fold increase in the limiting current density compared to a nanoparticle-based catalyst alone.
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Surface reconstruction of pure-Cu single-crystal electrodes under CO-reduction potentials in alkaline solutions: A study by seriatim ECSTM-DEMS

TL;DR: In this article, the authors showed that a polycrystalline Cu electrode kept in 0.1 M KOH at − 0.9 V (SHE), a potential very close to that for electrochemical CO reduction, underwent a two-step surface reconstruction, initially to Cu(111, or Cu(pc)-[Cu(111)], and terminally to either Cu(100, or CoCoCoCo-CoCo)-Cu(100).
Journal ArticleDOI

Selective Electrochemical Reduction of CO2 to Ethylene on Nanopores-Modified Copper Electrodes in Aqueous Solution

TL;DR: When used in electrolysis process, the as-prepared nanopores-modified electrodes can suppress the Faradaic efficiency toward methane to less than 1%, while keeping that of ethylene in a high level of 35% in aqueous 0.1 M KHCO3 solution under -1.3 V, thus revealing a remarkable selectivity toward ethylene production.
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