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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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High-Pressure CO Electroreduction at Silver Produces Ethanol and Propanol.

TL;DR: In this article, the authors investigated CO reduction at higher surface coverage (by increasing pressure) to ascertain if desorption effects can explain the discrepancy between density functional theory (DFT) and experimental results (ethanol vs no ethanol).
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Three-Dimensional Cathodes for Electrochemical Reduction of CO2: From Macro- to Nano-Engineering.

TL;DR: This work reviews the latest developments in experimental and modeling studies of three-dimensional cathodes towards high-performance electrochemical reduction of CO2, and the fabrication–microstructure–performance relationships of electrodes are examined from the macro- to nanoscale.
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Efficient and Selective Interplay Revealed: CO2 Reduction to CO over ZrO2 by Light with Further Reduction to Methane over Ni0 by Heat Converted from Light

TL;DR: In this paper, the reaction mechanism of CO2 photoreduction into methane was elucidated by time-course monitoring of the mass chromatogram, in situ FTIR spectroscopy, and in situ extended X-ray absorption fine structure (EXAFS).
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Reaction Selectivity for Plasmon-Driven Carbon Dioxide Reduction on Silver Clusters: A Theoretical Prediction

TL;DR: In this paper, density functional theory is employed to investigate the plasmon-driven CO2 reduction at the active sites of metallic silver clusters, and the results predict that CO2 prefers to adsorb at the bridge s...
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Electrocatalytic conversion of CO2 to hydrocarbon and alcohol products: Realities and prospects of Cu-based materials

TL;DR: In this article, the expectation, reality of the mechanism on Cu electrodes and its prospect to convert CO2 to aldehydes, hydrocarbon and alcohol products by a way of utilizing CO2 for industrial feedstocks.
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.
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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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