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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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Challenges and Opportunities in Electrocatalytic CO <sub>2</sub> Reduction to Chemicals and Fuels

TL;DR: In this article , the authors discuss practical challenges in the industrial chain that hamper the scaling-up deployment of the Electrocatalytic CO2 reduction (ECO2R) technology.
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Achieving highly selective electrochemical CO2 reduction to C2H4 on Cu nanosheets

TL;DR: In this paper , the authors demonstrate that the high activity and selectivity of CuO nanosheets originate from the edge sites on CuO nanoparticles with a coordinate number around 5 (4-6), which facilitates the formation of *CHO rather than *COH intermediate, meanwhile boosting the C C coupling reaction of *CO and *CHO intermediates, which are the critical steps for C2H4 formation.
Journal ArticleDOI

Boosting electrosynthesis of urea from N2 and CO2 by defective Cu-Bi

TL;DR: In this paper , the defective Cu-Bi catalyst was shown to offer a maximum urea concentration of 0.45 ± 0.06 mg L−1 and the largest faradaic efficiency of 8.7% ± 1.7%.
Journal ArticleDOI

Three-phase electrochemistry for green ethylene production

TL;DR: In this paper, the authors summarize the recent progresses on electrochemical ethylene production and present the principles for the design of gas-liquid-solid and gas-solid-solid three-phase interfaces.
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Interfacial O2 Accumulation Affects Microenvironment in Carbon-Based Electrocatalysts for H2O2 Production

TL;DR: In this article , the authors show that the oxygen-accumulation interface can not only provide more three phase contact points to improve the utilization efficiency of active sites but also increase the local pH, which stabilizes the intermediates and inhibits the protonation process within the reaction microenvironment, thus enabling a high H2O2 production selectivity.
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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