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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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Towards membrane-electrode assembly systems for CO2 reduction: a modeling study

TL;DR: In this article, a multiphysics model was developed to investigate the fundamental limitations of two MEA designs: one with gaseous feeds at both the anode and cathode (full-MEA), and the other with an aqueous anode feed (KHCO3 or KOH exchange solution) and a Gaseous cathode feed(exchange MEA).
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Rational catalyst design for N2 reduction under ambient conditions: Strategies towards enhanced conversion efficiency

TL;DR: Ammonia (NH3), one of the basic chemicals in most fertilizers and a promising carbon-free energy storage carrier, is typically synthesized via the Haber-Bosch process with high energy consumption as discussed by the authors.
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Branched Copper Oxide Nanoparticles Induce Highly Selective Ethylene Production by Electrochemical Carbon Dioxide Reduction

TL;DR: The initial branched copper oxide structure formed highly active domains with interfaces and junctions in-between during activation, which caused large surface area with high local pH leading to high selectivity and activity for ethylene production.
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Photoelectrochemical Synthesis of Ammonia on the Aerophilic-Hydrophilic Heterostructure with 37.8% Efficiency

TL;DR: In this paper, a unique aerophilic-hydrophilic heterostructured Si-based photocathode was designed for nitrogen-to-ammonia fixation in an acid electrolyte under mild conditions.
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Opportunities and Challenges for Catalysis in Carbon Dioxide Utilization

TL;DR: The environmental and societal consequences of the increasing levels of carbon dioxide in our atmosphere are among the most significant challenges society currently faces as discussed by the authors, and carbon dioxide utilisation is one of the most important challenges.
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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