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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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Tailoring the Surface and Interface Structures of Copper-Based Catalysts for Electrochemical Reduction of CO2 to Ethylene and Ethanol.

TL;DR: In this paper, the effects of surface and interface structures in Cu-based catalysts for CO2-to-ethylene/ethanol production are systematically discussed, and the guidance for the design of Cu based catalysts is provided for the highly efficient reduction of CO2.
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Uncovering the reaction mechanism behind CoO as active phase for CO2 hydrogenation

TL;DR: In this paper , the authors presented catalysts comprising of cobalt (oxide) nanoparticles stabilized on various support oxides for hydrocarbon production from carbon dioxide, and demonstrated that the activity and selectivity can be tuned by selection of the support oxide and cobalt oxidation state.
Journal ArticleDOI

Self-assembled Cuprous Coordination Polymer as a Catalyst for CO2 Electrochemical Reduction into C2 Products

TL;DR: In this article, the authors presented the electrochemical reduction of CO2 into C2 products such as ethylene and ethanol with metal complex catalysts, which is a significant challenge.
Journal ArticleDOI

Partial Coordination-Perturbed Bi-Copper Sites for Selective Electroreduction of CO2 to Hydrocarbons.

TL;DR: In this paper, a stable single-chain catalyst model system for electrochemical CO2 reduction reaction (CO2 RR) was designed and synthesized, which involves four homomorphic one-dimensional chain-like compounds.
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.
Journal ArticleDOI

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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