scispace - formally typeset
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.

read more

Citations
More filters
Journal ArticleDOI

Electrocatalytic CO 2 reduction towards industrial applications

TL;DR: In this article , a review of the electrocatalytic CO2 reduction reaction (eCO2RR) for industrial applications is presented, focusing on potential industrial catalysts and potential industrial products.
Journal ArticleDOI

High‐Rate and Selective CO2 Electrolysis to Ethylene via Metal–Organic‐Framework‐Augmented CO2 Availability

Abstract: High‐rate conversion of carbon dioxide (CO2) to ethylene (C2H4) in the CO2 reduction reaction (CO2RR) requires fine control over the phase boundary of the gas diffusion electrode (GDE) to overcome the limit of CO2 solubility in aqueous electrolytes. Here, a metal–organic framework (MOF)‐functionalized GDE design is presented, based on a catalysts:MOFs:hydrophobic substrate materials layered architecture, that leads to high‐rate and selective C2H4 production in flow cells and membrane electrode assembly (MEA) electrolyzers. It is found that using electroanalysis and operando X‐ray absorption spectroscopy (XAS), MOF‐induced organic layers in GDEs augment the local CO2 concentration near the active sites of the Cu catalysts. MOFs with different CO2 adsorption abilities are used, and the stacking ordering of MOFs in the GDE is varied. While sputtering Cu on poly(tetrafluoroethylene) (PTFE) (Cu/PTFE) exhibits 43% C2H4 Faradaic efficiency (FE) at a current density of 200 mA cm−2 in a flow cell, 49% C2H4 FE at 1 A cm−2 is achieved on MOF‐augmented GDEs in CO2RR. MOF‐augmented GDEs are further evaluated in an MEA electrolyzer, achieving a C2H4 partial current density of 220 mA cm−2 for CO2RR and 121 mA cm−2 for the carbon monoxide reduction reaction (CORR), representing 2.7‐fold and 15‐fold improvement in C2H4 production rate, compared to those obtained on bare Cu/PTFE.
Journal ArticleDOI

Probing dissolved CO2(aq) in aqueous solutions for CO2 electroreduction and storage

TL;DR: In this paper , microscale infrared spectroscopy was used for in situ dynamic quantification of CO2(aq) in aqueous solutions, and the quantized CO 2(g) rotational state transitions were observed to quench for CO2, accompanied by increased H2O IR absorption.
Journal ArticleDOI

Photocatalytic Hedgehog Particles for High Ionic Strength Environments.

TL;DR: In this article, hedgehog particles with semiconductor nanoscale spikes display enhanced stability in solutions of monovalent/divalent salts in both aqueous and hydrophobic media.
References
More filters
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.
Journal ArticleDOI

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.
Journal ArticleDOI

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.
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.
Related Papers (5)