Journal ArticleDOI
CO2 electroreduction to ethylene via hydroxide-mediated copper catalysis at an abrupt interface
Cao-Thang Dinh,Thomas Burdyny,Golam Kibria,Ali Seifitokaldani,Christine M. Gabardo,F. Pelayo García de Arquer,Amirreza Kiani,Jonathan P. Edwards,Phil De Luna,Oleksandr S. Bushuyev,Chengqin Zou,Chengqin Zou,Rafael Quintero-Bermudez,Yuanjie Pang,David Sinton,Edward H. Sargent +15 more
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
Looking Back and Looking Ahead in Electrochemical Reduction of CO2
TL;DR: This personal account particularly focuses on the recent progress that has been achieved by the Ertl Center and a number of groups in South Korea that becomes one of the larger CO2 emitters.
Journal ArticleDOI
Hydrophobic 1-octadecanethiol functionalized copper catalyst promotes robust high-current CO2 gas-diffusion electrolysis
Liangyao Xue,Xue Feng Wu,Yuanwei Liu,Beibei Xu,Xuelu Wang,Sheng Dai,Peng Fei Liu,Hua Gui Yang +7 more
TL;DR: In this paper, the hydrophobic 1-octadecanethiol molecular was functionalized over the Cu catalyst layer of the GDE, which simultaneously stabilizes the GDL and exposes abundant active solid-liquid-gas three-phase interfaces.
Journal ArticleDOI
Beyond catalytic materials: Controlling local gas/liquid environment in the catalyst layer for CO2 electrolysis
TL;DR: In this paper , the microenvironment in the catalyst layer for CO2 electrolysis, including typical mass transport models for CO 2 reduction in H-type cells and GDE flow cells, the effect of a hydrophobic microenvironment on CO2 mass transport and catalytic performance, and the formation of a gas/liquid balance and solid-liquid-gas interfaces are discussed.
Journal ArticleDOI
Electrochemical carbon dioxide reduction on copper–zinc alloys: ethanol and ethylene selectivity analysis
TL;DR: In this article , the effect of local atomic arrangement of CuZn alloys was demonstrated on enhanced ethanol selectivity from CO 2 RR and supported by density functional theory (DFT) calculations.
Journal ArticleDOI
Energy- and carbon-efficient CO_2/CO electrolysis to multicarbon products via asymmetric ion migration–adsorption
Adnan Ozden,Jian Li,Sharath Kandambeth,Xiao-yan Li,Shijie Liu,Osama Shekhah,Pengfei Ou,Y. Zou Finfrock,Ya-Kun Wang,Tartela Alkayyali,F. Pelayo García de Arquer,Vinayak S. Kale,Prashant M. Bhatt,Alexander H. Ip,Mohamed Eddaoudi,Edward H. Sargent,David Sinton +16 more
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.
Georg Kresse,Jürgen Furthmüller +1 more
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
Georg Kresse,Daniel P. Joubert +1 more
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
Graeme Henkelman,Hannes Jónsson +1 more
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)
Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte
Stephanie A. Nitopi,Erlend Bertheussen,Søren Bertelsen Scott,Xinyan Liu,Albert K. Engstfeld,Albert K. Engstfeld,Sebastian Horch,Brian Seger,Ifan E. L. Stephens,Ifan E. L. Stephens,Karen Chan,Karen Chan,Christopher Hahn,Christopher Hahn,Jens K. Nørskov,Jens K. Nørskov,Jens K. Nørskov,Thomas F. Jaramillo,Thomas F. Jaramillo,Ib Chorkendorff +19 more