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
Advantages of CO over CO2 as reactant for electrochemical reduction to ethylene, ethanol and n-propanol on gas diffusion electrodes at high current densities
N.S. Romero Cuellar,N.S. Romero Cuellar,Kerstin Wiesner-Fleischer,Maximilian Fleischer,A. Rucki,Olaf Hinrichsen +5 more
TL;DR: In this article, the authors used gas diffusion electrodes in a flow cell for the electrochemical reduction of CO2 and CO towards C2 and C3 products, and showed that with CO as the reactant, higher current densities can be achieved at lower working electrode potentials compared to CO2 as the reactionant.
Journal ArticleDOI
Metal-based heterogeneous electrocatalysts for reduction of carbon dioxide and nitrogen: mechanisms, recent advances and perspective
Jun-Hao Zhou,Ya-Wen Zhang +1 more
TL;DR: In this paper, the similarities and differences between CO2RR and NRR were discussed in the following aspects: fundamental theory of the reaction mechanisms and the corresponding catalyst design principles; reaction systems and product analysis methods; recent advances in heterogeneous electrocatalysts synthesized from different metals with various compositions, structures and morphologies.
Journal ArticleDOI
Electrochemical Real-Time Mass Spectrometry (EC-RTMS): Monitoring Electrochemical Reaction Products in Real Time.
Peyman Khanipour,Peyman Khanipour,Mario Löffler,Mario Löffler,Andreas M. Reichert,Andreas M. Reichert,Felix T. Haase,Felix T. Haase,Karl Johann Jakob Mayrhofer,Karl Johann Jakob Mayrhofer,Ioannis Katsounaros +10 more
TL;DR: The electrochemical real time mass spectrometry (EC-RTMS) approach is used to determine the products of the CO2 reduction reaction (CO2 RR) during potential step or sweep experiments on pristine and in-situ anodized copper.
Journal ArticleDOI
Structure‐Tunable Copper–Indium Catalysts for Highly Selective CO2 Electroreduction to CO or HCOOH
TL;DR: For the first time, it is reported that by varying the metal ratio, the catalyst can be tuned from a core-shell structure that selectively produces CO to a well-mixed structure that prefers HCOOH production.
Journal ArticleDOI
Two-Dimensional SnO2 Nanosheets for Efficient Carbon Dioxide Electroreduction to Formate
TL;DR: In this paper, two-dimensional SnO2 nanosheet (∼3 nm in diameter) was used for electrocatalytic reduction of CO2 to liquid fuels, which is a promising strategy to store the intermittent renewable energies into high value chemicals.
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