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
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
TL;DR: A broad and historical view of different aspects and their complex interplay in CO2R catalysis on Cu is taken, with the purpose of providing new insights, critical evaluations, and guidance to the field with regard to research directions and best practices.
Journal ArticleDOI
What would it take for renewably powered electrosynthesis to displace petrochemical processes
Phil De Luna,Phil De Luna,Phil De Luna,Christopher Hahn,Christopher Hahn,Drew Higgins,Drew Higgins,Drew Higgins,Shaffiq Jaffer,Thomas F. Jaramillo,Thomas F. Jaramillo,Edward H. Sargent +11 more
TL;DR: A comparative analysis of electrocatalyst and carbon emissions assessment of CO2 products such as ethylene, ethanol, and carbon monoxide shows that electrocatalytic production has the potential to yield the greatest reduction in carbon emissions, provided that a steady supply of clean electricity is available.
Journal ArticleDOI
Advances and challenges in understanding the electrocatalytic conversion of carbon dioxide to fuels
Yuvraj Y. Birdja,Yuvraj Y. Birdja,Elena Pérez-Gallent,Marta C. Figueiredo,Marta C. Figueiredo,Adrien J. Göttle,Federico Calle-Vallejo,Federico Calle-Vallejo,Marc T. M. Koper +8 more
TL;DR: In this article, the authors review recent advances and challenges in the understanding of electrochemical CO2 reduction and discuss existing models for the initial activation of CO2 on the electrocatalyst and their importance for understanding selectivity.
Journal ArticleDOI
Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products
TL;DR: In this article, the authors discuss strategies to achieve high selectivity towards multicarbon products via rational catalyst and electrolyte design, focusing on findings extracted from in situ and operando characterizations.
Journal ArticleDOI
CO2 electrolysis to multicarbon products at activities greater than 1 A cm−2
F. Pelayo García de Arquer,Cao-Thang Dinh,Adnan Ozden,Joshua Wicks,Christopher McCallum,Ahmad R. Kirmani,Dae-Hyun Nam,Christine M. Gabardo,Ali Seifitokaldani,Xue Wang,Yuguang C. Li,Fengwang Li,Jonathan P. Edwards,Lee J. Richter,Steven J. Thorpe,David Sinton,Edward H. Sargent +16 more
TL;DR: A catalyst:ionomer bulk heterojunction (CIBH) architecture that decouples gas, ion, and electron transport and achieves CO2 electroreduction on copper in 7 M potassium hydroxide electrolyte with an ethylene partial current density at 45% cathodic energy efficiency.
References
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Journal ArticleDOI
Tuning the Selectivity of Carbon Dioxide Electroreduction toward Ethanol on Oxide-Derived CuxZn Catalysts
TL;DR: In this article, the selectivity of CO2 reduction toward ethanol could be tuned by introducing a cocatalyst to generate an in situ source of mobile CO reactant, which can be used as catalysts.
Journal ArticleDOI
High Selectivity for Ethylene from Carbon Dioxide Reduction over Copper Nanocube Electrocatalysts
TL;DR: The ability of the cubic nanostructure to so strongly favor multicarbon product formation from CO2 reduction, and in particular ethylene over methane, is unique to this surface and is an important step toward developing a catalyst that has exclusive selectivity for multicarbon products.
Journal ArticleDOI
Identification of Possible Pathways for C-C Bond Formation during Electrochemical Reduction of CO2: New Theoretical Insights from an Improved Electrochemical Model.
TL;DR: The electrochemical model reported here is simple, fairly easy to implement, and involves only a small increase in computational cost over calculations neglecting the effects of the electrolyte and the applied field, Therefore, it can be used to study theeffects of applied potential and electrolyte composition on the energetics of surface reactions for a wide variety of electrochemical reactions.
Journal ArticleDOI
Electrochemical Reduction of CO2 Using Copper Single-Crystal Surfaces: Effects of CO* Coverage on the Selective Formation of Ethylene
TL;DR: In this article, the authors elucidated a fundamental reason underlying the selectivity of CO2 reduction toward C2 products by studying its reactivity on Cu(100), Cu(111), and Cu(110) single-crystal surfaces.
Journal ArticleDOI
Copper nanoparticle ensembles for selective electroreduction of CO2 to C2–C3 products
TL;DR: This work presents a copper-based catalyst, formed in situ from an ensemble of nanoparticles, that is able to selectively generate C2–C3 products at low overpotentials with good stability, where their efficient formation has been difficult to achieve.
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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