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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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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

Effects of electrolyte, catalyst, and membrane composition and operating conditions on the performance of solar-driven electrochemical reduction of carbon dioxide

TL;DR: This article provides useful guidelines for minimizing polarization losses in solar-driven CO2R electrochemical cells and a method for predicting polarization losses and obtaining kinetic overpotentials from measured partial current densities.
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Three-dimensional porous hollow fibre copper electrodes for efficient and high-rate electrochemical carbon dioxide reduction

TL;DR: The design of a porous hollow fibre copper electrode with a compact three-dimensional geometry, which provides a large area, three-phase boundary for gas–liquid reactions, which may inspire the development of new types of microtubular electrodes for electrochemical processes in which at least one gas-phase reactant is involved, such as in fuel cell technology.
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Stable and selective electrochemical reduction of carbon dioxide to ethylene on copper mesocrystals

TL;DR: In this article, a stable and selective electrochemical reduction of carbon dioxide to ethylene was achieved using copper mesocrystal catalysts in 0.1 M KHCO3 using high resolution transmission electron microscopy.
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Morphology-Directed Selective Production of Ethylene or Ethane from CO2 on a Cu Mesopore Electrode

TL;DR: It is demonstrated that C2 chemical selectivity can be tuned by systematically altering the morphology and supported by computational simulations, it is proved that nanomorphology can change the local pH and retention time of key intermediates by confining the chemicals inside the pores.
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Subsurface oxide plays a critical role in CO2 activation by Cu(111) surfaces to form chemisorbed CO2, the first step in reduction of CO2

TL;DR: This work reveals the essential first step for activating CO2 on a Cu surface, in particular, highlighting the importance of copper suboxide and the critical role of water, and provides fresh insights into how to design improved carbon dioxide reduction catalysts.
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