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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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Citations
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Journal ArticleDOI

Copper Nanocubes for CO2 Reduction in Gas Diffusion Electrodes.

TL;DR: In this article, the effect of nanoparticle shape on the electrocatalysis of CO2 reduction by using gas-diffusion electrodes (GDEs) and flowing alkaline catholytes was investigated.
Journal ArticleDOI

Hierarchical Copper with Inherent Hydrophobicity Mitigates Electrode Flooding for High-Rate CO2 Electroreduction to Multicarbon Products.

TL;DR: In this paper, a bioinspired copper catalyst on a gas diffusion layer that mimics the unique hierarchical structuring of Setaria's hydrophobic leaves was proposed, which can not only trap more CO close to the active copper surface but also effectively resist electrolyte flooding even under high-rate operation.
Journal ArticleDOI

Fundamentals of Electrochemical CO2 Reduction on Single-Metal-Atom Catalysts

TL;DR: In this paper, the authors proposed an approach to produce valuable products from CO2 and to store intermittent renewable energy for storing and storing the earth-scale human waste and CO2.
Journal ArticleDOI

In Situ Observation of the pH Gradient near the Gas Diffusion Electrode of CO2 Reduction in Alkaline Electrolyte.

TL;DR: A continuous-flow Raman electrochemical cell is developed that enables the first experimental study of the local pH near a CO2 reduction gas diffusion electrode under reaction conditions, and verifies that the nominal overpotential reduction from using alkaline electrolyte originates from the Nernst potential of the pH gradient layer at the cathode/electrolyte interface.
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.
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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