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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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Evidence for product-specific active sites on oxide-derived Cu catalysts for electrochemical CO2 reduction

TL;DR: In this article, it was shown that oxide-derived Cu catalysts have three different types of active sites for C-C coupled products, one that produces ethanol and acetate, another that produces ethylene and yet another producing 1-propanol.
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Current progress in electrocatalytic carbon dioxide reduction to fuels on heterogeneous catalysts

TL;DR: In this article, the authors summarized the current research progress in the electrocatalytic reduction of CO2 to fuels on heterogeneous catalysts and provided effective guidance for the design of effective catalysts with high activity, product selectivity, faradaic efficiency, and stability.
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Catalyst–electrolyte interface chemistry for electrochemical CO2 reduction

TL;DR: The current understanding of the catalyst-electrolyte interface and its effect on the CO2 electroreduction activity is discussed and extensively review previous studies on controlling organic modulators, electrolyte ions, electrode structures, as well as the three-phase boundary at the catalyst.
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An industrial perspective on catalysts for low-temperature CO2 electrolysis

TL;DR: In this article, the key advances in nanocatalysts that have led to the impressive electrochemical conversion of CO2 to useful products and provides benchmarks that others can use to compare their results.
Journal ArticleDOI

General technoeconomic analysis for electrochemical coproduction coupling carbon dioxide reduction with organic oxidation

TL;DR: The analysis highlights the promise that coupling the carbon dioxide reduction reaction with the value-added organic oxidation reaction can secure significant economic feasibility, and develops a fully automated process synthesis framework to guide process simulations.
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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