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
Reads0
Chats0
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
Ga doping disrupts C-C coupling and promotes methane electroproduction on CuAl catalysts
Armin Sedighian Rasouli,Xue Wang,Joshua Wicks,Cao-Thang Dinh,Jehad Abed,Fengying Wu,Sung Fu Hung,Koen Bertens,Jianan Erick Huang,Edward H. Sargent +9 more
TL;DR: In this paper , the effect of doping CuAl, a material at the top of the CO2RR activity and selectivity volcano plot, with elements having low ∗CO binding energies: Au, Zn, and Ga.
Journal ArticleDOI
Solar-powered synthesis of hydrocarbons from carbon dioxide and water.
TL;DR: Promoting the efficient and selective formation of hydrocarbons of high value and utility requires a highly integrated approach in which electrocatalysts, electrolytes, cell parameters, and light-harvesting assemblies are optimized to work together.
Journal ArticleDOI
Facet-selective deposition of ultrathin Al2O3 on copper nanocrystals for highly stable CO2 electroreduction to ethylene
Hui Li,Peiping Yu,Renbo Lei,Feipeng Yang,Peng Wen,Xiao Ma,Guosong Zeng,Jinghua Guo,Francesca M. Toma,Yejun Qiu,Scott M. Geyer,Xinwei Wang,Tao Cheng,Walter S. Drisdell +13 more
TL;DR: In this paper, the authors used the facet-selective atomic layer deposition (FS-ALD) technique to selectively cover the (111) surface of Cu nanocrystals with ultrathin Al2 O3 to increase the exposed facet ratio of (100)/(111), resulting in a faradaic efficiency ratio of C2 H4 /CH4 for overcoated Cu NCs 22 times higher than that for pure CU NCs.
Journal ArticleDOI
Visualizing highly selective electrochemical CO2 reduction on a molecularly dispersed catalyst
TL;DR: In this paper, an in-situ, high-resolution, and high-speed microscale visualization technique is applied to observe the generation and detachment of the CO2RR products (CO and H2) on the electrode coated with molecularly dispersed electrocatalyst of methoxy group functionalized nickel phthalocyanine (NiPc-OMe MDE).
Journal ArticleDOI
Mechanistic routes toward C<sub>3</sub> products in copper-catalysed CO<sub>2</sub> electroreduction
Xiaoyu Li,O. P. Bychkov,Murat Altunkaynak[1] Umut Gül[2] Latife Canatan[3] İbrahim Daşkın[4] Gürsel Kütük[5] +2 more
TL;DR: In this article , the mechanistic insights of CO 2 electrochemical reduction on Cu materials up to C 3 fragments are investigated by combining experiments and theory, and the results show that CO 2 can be used to reduce Cu materials.
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