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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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Conversion of Bicarbonate to Formate in an Electrochemical Flow Reactor

TL;DR: In this paper, a CO2 reduction studies typically supply CO2 to the cathode as a gas or dissolved in aqueous media, and these feedstocks present challenges when scaling a CO 2 electrolyzer: gaseou...
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In Situ Formation of Nano Ni-Co Oxyhydroxide Enables Water Oxidation Electrocatalysts Durable at High Current Densities.

TL;DR: In this paper, a novel synthesis of nanocrystalline Ni-Co-Se using ball milling at cryogenic temperature is reported, and the resulting electrocatalyst exhibits an overpotential of 279 mV at 0.5 A cm-2 and 329mV at 1 A cm 2 and sustained performance for 500 h.
Journal ArticleDOI

Heterogeneous catalysts for catalytic CO2 conversion into value-added chemicals

TL;DR: In this article, a review of the heterogeneous catalysts used for the gas-phase reaction or electrochemical reactions are discussed, because the liquid phase reaction and photocatalytic reaction typically suffer from low productivity and poor durability.
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PdAg bimetallic electrocatalyst for highly selective reduction of CO 2 with low COOH* formation energy and facile CO desorption

TL;DR: In this paper, the PdAg bimetallic catalyst with Ag-terminated surface was designed to circumvent the drawbacks of sole Pd and Ag. Density functional theory (DFT) calculations reveal that the Agterminated pdAg surface features a lowered formation energy for COOH* and weakened adsorption for CO*, which both contribute to the enhanced performance for CO2 reduction.
Journal ArticleDOI

N-doped reduced graphene oxide supported Cu2O nanocubes as high active catalyst for CO2 electroreduction to C2H4

TL;DR: In this paper, a facile method to in situ load cuprous oxide (Cu2O) nanocubes on nitrogen doped reduced graphene oxide (NRGO) to fabricate a Cu2O/NRGO composite under ambient conditions, which exits a high faradaic efficiency of ethylene (19.7%) at −1.4
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.
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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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