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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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Bi2O3 Nanosheets Grown on Carbon Nanofiber with Inherent Hydrophobicity for High-Performance CO2 Electroreduction in a Wide Potential Window.

TL;DR: In this paper, the Bi2O3 nanosheets (NSs) with inherent hydrophobicity achieved a peak formate current density of 102.1 mA cm-2 and high formate Faradaic efficiency of >93% over a very wide potential window of 1000 mV.
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Hierarchical micro/nanostructured silver hollow fiber boosts electroreduction of carbon dioxide

TL;DR: In this paper , a hierarchical micro/nanostructured silver hollow fiber electrode that reduces CO2 to CO with a faradaic efficiency of 93% and a current density of 1.26 A · cm-2 at a potential of -0.83 V vs. RHE was reported.
Journal ArticleDOI

Mass transfer effect to electrochemical reduction of CO2: Electrode, electrocatalyst and electrolyte

TL;DR: In this article , the authors comprehensively reviewed development related to mass transfer study of CO2, including the mechanism of mass transfer of CO 2, and main factors (electrodes, electrocatalysts and electrolytes) on two-phase or multi-phase interface during eCO2RR.
Journal ArticleDOI

Catalytic Hybrid Electrocatalytic/Biocatalytic Cascades for Carbon Dioxide Reduction and Valorization

Abstract: Carbon dioxide, as a greenhouse gas, has a critical impact on global climate change. Hence, reducing its emissions and/or transforming it into value-added chemicals is of paramount importance to so...
Journal ArticleDOI

Syngas electrosynthesis using self-supplied CO2 from photoelectrocatalytic pollutant degradation

TL;DR: In this article, a single-chamber based two-electrode system was used to synthesize syngas using self-supplied CO2 from photoelectrocatalytic pollutant oxidation.
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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