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
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Journal ArticleDOI
Hydroxide Is Not a Promoter of C2+ Product Formation in the Electrochemical Reduction of CO on Copper
TL;DR: It is demonstrated that higher concentrations of cations (Na + ), rather than OH - , exert the main promotional effect on the production of C 2+ products by systematically varying the concentration of Na + and OH - at identical absolute electrode potential.
Journal ArticleDOI
Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction.
Peng Zhu,Chuan Xia,Chun-Yen Liu,Kun Jiang,Guanhui Gao,Xiao Zhang,Yang Xia,Yongjiu Lei,Husam N. Alshareef,Thomas P. Senftle,Haotian Wang,Haotian Wang +11 more
TL;DR: In this paper, the authors demonstrate a direct and continuous generation of pure acetic acid solutions via electrochemical CO reduction by coupling rational designs in a Cu catalyst and porous solid electrolyte (PSE) reactor.
Journal ArticleDOI
Oxygen induced promotion of electrochemical reduction of CO 2 via co-electrolysis.
Ming He,Chunsong Li,Haochen Zhang,Xiaoxia Chang,Jingguang G. Chen,William A. Goddard,Mu Jeng Cheng,Bingjun Xu,Qi Lu +8 more
TL;DR: It is found that co-electrolysis of CO2 with O2 can enhance copper’s catalytic activities and is a promising strategy to introduce catalytically active species in electrocatalysis.
Journal ArticleDOI
Electronic Effects Determine the Selectivity of Planar Au–Cu Bimetallic Thin Films for Electrochemical CO2 Reduction
Kai Liu,Ming Ma,Longfei Wu,Marco Valenti,Drialys Cardenas-Morcoso,Jan P. Hofmann,Juan Bisquert,Sixto Gimenez,Wilson A. Smith +8 more
TL;DR: The formation of CO and HCOO– as main CO2 reduction products on planar Au–Cu alloys followed the shift of the d-band center, which indicates that the electronic effect is the major governing factor for the electrocatalytic activity ofCO2 reduction on Au– Cu bimetallic thin films.
Journal ArticleDOI
A Planar, Conjugated N 4 -Macrocyclic Cobalt Complex for Heterogeneous Electrocatalytic CO 2 Reduction with High Activity
TL;DR: A novel planar and conjugated N4-macrocyclic cobalt complex (Co(II)CPY) derived from phenanthroline subunits is prepared, which delivers high activity for heterogeneous CO 2 electrocatalysis to CO in an aqueous medium and outperforms most of the metal complexes reported so far.
References
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Generalized Gradient Approximation Made Simple
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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