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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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Journal ArticleDOI

Electrochemical Reduction of CO2 on Metal-Nitrogen-Doped Carbon Catalysts

TL;DR: The electrochemical CO2 reduction reaction (CO2RR) is a promising technology for converting waste CO2 into chemicals which could be used as feedstock for the chemical industry or as synthetic fuels.
Journal ArticleDOI

Stability and Degradation Mechanisms of Copper‐Based Catalysts for Electrochemical CO 2 Reduction

TL;DR: In this article, the recent progress on understanding the stability of copper-based catalysts is summarized, along with the very few proposed degradation mechanisms, and a perspective on the topic is given.
Journal ArticleDOI

Transforming the carbon economy: challenges and opportunities in the convergence of low-cost electricity and reductive CO2 utilization

TL;DR: In this paper, the authors assess and characterize the top technical barriers for utilizing renewable electricity for CO2 reduction across five different conversion approaches (direct electrochemical, direct bioelectrochemical, indirect non-thermal plasma, indirect bioelectron, and indirect thermochemical) under state-of-technology conditions, outline the R&D needs to overcome each barrier, and identify the most promising C1-C3 hydrocarbons and oxygenates based on their relative ease of formation, economic viability, CO2 utilization potential, and energy storage capacity.
Journal ArticleDOI

Efficient wettability-controlled electroreduction of CO2 to CO at Au/C interfaces.

TL;DR: The Cassie-Wenzel coexistence state is demonstrated to be the ideal three phase structure for continuous CO2 supply from gas phase to Au active sites at high current densities and the pivotal role of interfacial structure for the stabilization of the interfacial CO2 concentration during CO2RR is quantitatively analysed.
Journal ArticleDOI

Electrochemical Carbon Monoxide Reduction on Polycrystalline Copper: Effects of Potential, Pressure, and pH on Selectivity toward Multicarbon and Oxygenated Products

TL;DR: In this article, a planar polycrystalline copper as an electrocatalyst for CO reduction under alkaline conditions was used to investigate the surface reactivity of CO, which is a key intermediate during electrochemical CO2 reduction.
References
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Journal ArticleDOI

Generalized Gradient Approximation Made Simple

TL;DR: A simple derivation of a simple GGA is presented, in which all parameters (other than those in LSD) are fundamental constants, and only general features of the detailed construction underlying the Perdew-Wang 1991 (PW91) GGA are invoked.
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Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set.

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From ultrasoft pseudopotentials to the projector augmented-wave method

TL;DR: In this paper, the formal relationship between US Vanderbilt-type pseudopotentials and Blochl's projector augmented wave (PAW) method is derived and the Hamilton operator, the forces, and the stress tensor are derived for this modified PAW functional.
Journal ArticleDOI

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

TL;DR: An improved way of estimating the local tangent in the nudged elastic band method for finding minimum energy paths is presented, and examples given where a complementary method, the dimer method, is used to efficiently converge to the saddle point.
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A grid-based Bader analysis algorithm without lattice bias

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