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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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Advantages of CO over CO2 as reactant for electrochemical reduction to ethylene, ethanol and n-propanol on gas diffusion electrodes at high current densities

TL;DR: In this article, the authors used gas diffusion electrodes in a flow cell for the electrochemical reduction of CO2 and CO towards C2 and C3 products, and showed that with CO as the reactant, higher current densities can be achieved at lower working electrode potentials compared to CO2 as the reactionant.
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Metal-based heterogeneous electrocatalysts for reduction of carbon dioxide and nitrogen: mechanisms, recent advances and perspective

TL;DR: In this paper, the similarities and differences between CO2RR and NRR were discussed in the following aspects: fundamental theory of the reaction mechanisms and the corresponding catalyst design principles; reaction systems and product analysis methods; recent advances in heterogeneous electrocatalysts synthesized from different metals with various compositions, structures and morphologies.
Journal ArticleDOI

Electrochemical Real-Time Mass Spectrometry (EC-RTMS): Monitoring Electrochemical Reaction Products in Real Time.

TL;DR: The electrochemical real time mass spectrometry (EC-RTMS) approach is used to determine the products of the CO2 reduction reaction (CO2 RR) during potential step or sweep experiments on pristine and in-situ anodized copper.
Journal ArticleDOI

Structure‐Tunable Copper–Indium Catalysts for Highly Selective CO2 Electroreduction to CO or HCOOH

TL;DR: For the first time, it is reported that by varying the metal ratio, the catalyst can be tuned from a core-shell structure that selectively produces CO to a well-mixed structure that prefers HCOOH production.
Journal ArticleDOI

Two-Dimensional SnO2 Nanosheets for Efficient Carbon Dioxide Electroreduction to Formate

TL;DR: In this paper, two-dimensional SnO2 nanosheet (∼3 nm in diameter) was used for electrocatalytic reduction of CO2 to liquid fuels, which is a promising strategy to store the intermittent renewable energies into high value chemicals.
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.
Journal ArticleDOI

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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