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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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Electroenzymatic CO2 Fixation Using Redox Polymer/Enzyme-Modified Gas Diffusion Electrodes

TL;DR: In this article, the fabrication of gas diffusion electrodes modified with polymer/enzyme layers for electroenzymatic CO2 fixation is described, using a metal-free organic low-potential viologen-modified polymer.
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Synergized Cu/Pb Core/Shell Electrocatalyst for High-Efficiency CO2 Reduction to C2+ Liquids.

TL;DR: In this article, the authors demonstrate that the strong synergy between Cu core and ultrathin lead (Pb) shell (0.7 nm) in the Cu/Pb core/shell nanocrystals significantly boosts the electrocatalytic reduction of CO2 toward C2+ products (products with at least two carbon atoms).
Journal ArticleDOI

A systematic analysis of Cu-based membrane-electrode assemblies for CO2 reduction through multiphysics simulation

TL;DR: In this paper, the performance of a copper-based membrane-electrode assembly (Cu-MEA) was investigated for the reduction of CO2 to C2+ products, while maintaining high current densities.
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Advanced manufacturing for electrosynthesis of fuels and chemicals from CO2

TL;DR: In this article, the authors demonstrate AM for rapid development and testing for improved performance for the carbon dioxide reduction reaction across an evolution of vapor-fed reactor designs, and define a dimensionless number to identify mass transport regimes by exploring the impact of hypothesized underlying mass transport mechanisms.
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.

TL;DR: An efficient scheme for calculating the Kohn-Sham ground state of metallic systems using pseudopotentials and a plane-wave basis set is presented and the application of Pulay's DIIS method to the iterative diagonalization of large matrices will be discussed.
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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.
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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.
Journal ArticleDOI

A grid-based Bader analysis algorithm without lattice bias

TL;DR: This paper describes how accurate off-lattice ascent paths can be represented with respect to the grid points, and maintains the efficient linear scaling of an earlier version of the algorithm, and eliminates a tendency for the Bader surfaces to be aligned along the grid directions.
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