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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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Journal ArticleDOI

Transient Effects Caused by Gas Depletion during Carbon Dioxide Electroreduction.

TL;DR: It is concluded that CO2 depletion causes a strong decay in the electrochemical reaction efficiency, and pH is suggested as an accurate and indirect means to measure CO2 concentration in a liquid electrolyte.
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CO2-free high-purity ethylene from electroreduction of CO2 with 4% solar-to-ethylene and 10% solar-to-carbon efficiencies

TL;DR: In this article , an aqueous flow-through electrochemical cell was developed to enhance the activity and selectivity of C2H4 on a three-dimensional (3D) Cu mesh electrode by applying square wave oscillating potentials.
Journal ArticleDOI

First-principles study of N2O decomposition on (001) facet of perovskite LaBO3 (B = Mn, Co, Ni)

TL;DR: In this article, density functional theory was used to investigate the N2O molecule decomposition mechanism on LaBO3 perovskites in terms of thermodynamics and kinetics.
Journal ArticleDOI

Bicarbonate Electroreduction to Multicarbon Products Enabled by Cu/Ag Bilayer Electrodes and Tailored Microenviroments

TL;DR: In this paper , a bicarbonate electrolyzer can achieve the direct conversion of CO2 capture solutions to multicarbon (C2+) products (i.e., acetate, ethylene, ethanol, propanol) on rationally designed Cu/Ag bilayer electrodes with bilayer cation-and anion conducting ionomers.
Journal ArticleDOI

Hydrophobic Electrode Design for CO2 Electroreduction in a Microchannel Reactor.

TL;DR: In this article , a hydrophobic polytetrafluoroethylene (PTFE)-doped Ag nanocatalyst on a Zn rod was synthesized through a facile galvanic replacement of 2Ag++Zn → 2Ag + Zn2+.
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.
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

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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