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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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Electrooxidation of saturated C1-C3 primary alcohols on platinum: Potential-resolved product analysis with electrochemical real-time mass spectrometry (EC-RTMS)

TL;DR: In this paper, the authors provide details on the interpretation of data for electrochemical real-time mass spectrometry (EC-RTMS) and on the assignment of mass signals to reaction products by studying three model reactions.
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Microenvironments of Cu Catalyst in Zero-gap Membrane Electrode Assembly for Efficient CO2 Electrolysis to C2+ Products

TL;DR: A zero-gap membrane-electrode assembly (MEA) electrolyzer is a promising design for electrochemical CO2 reduction reactions (eCO2RR) where gaseous CO2 is directly fed without catholyte.
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Electrochemical C-N coupling of CO2 and nitrogenous small molecules for the electrosynthesis of organonitrogen compounds.

TL;DR: In this paper , a comprehensive review on the electrosynthesis of high value-added organonitrogens from the abundant CO2 and nitrogenous small molecules (N2, NO, NO2-, NO3-, NH3), together with the current challenges and future opportunities are discussed.
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Reviewing the impact of halides on electrochemical CO 2 reduction

TL;DR: A comprehensive review of the role and mechanism of halide ions in the CO 2 reduction reaction can help better guide the future design of efficient electrocatalysts as discussed by the authors .
Journal ArticleDOI

Electrochemical CO2 Reduction on Polycrystalline Copper by Modulating Proton Transfer with Fluoropolymer Composites

TL;DR: In this paper , a 15 μm Nafion overlayer was used to control proton transfer in an acetonitrile/bicarbonate electrolyte, resulting in a higher yield of total carbon-containing products than an analogous unmodified Cu electrode.
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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