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CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface

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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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Recent Development of Electrocatalytic CO2 Reduction Application to Energy Conversion

TL;DR: A clear and innovative insight is provided into the entire reaction process of CRR, guiding the new electrocatalysts design, state-of-the-art analysis technique application, and reaction system innovation.
Journal ArticleDOI

Two-step electrochemical reduction of CO2 towards multi-carbon products at high current densities

TL;DR: In this article, two-step electrochemical reduction of CO2 is investigated as an alternative to increase selectivity towards C2 and C3 products in a cascade electrocatalytic operation, where CO is produced in a first step and subsequently reduced to multi-carbon products with significantly higher Faradaic efficiencies compared to a one-step process.
Journal ArticleDOI

Design Strategies for Markedly Enhancing Energy Efficiency in Electrocatalytic CO2 Reduction Reaction

TL;DR: In this paper , the authors proposed a promising approach to ameliorate the global warming and energy crisis by using electrocatalytic CO2 reduction reaction (CO2RR).
Journal ArticleDOI

Revealing the Predominant Surface Facets of Rough Cu Electrodes under Electrochemical Conditions

TL;DR: In this article, metal electrodes with rough surfaces are often found to convert CO or CO2 to hydrocarbons and oxygenates with high selectivity and at high reaction rates in comparison with their smooth counterpart.
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.

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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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