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
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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
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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
Electroreduction of carbon dioxide to hydrocarbons using bimetallic Cu-Pd catalysts with different mixing patterns
Sichao Ma,Masaaki Sadakiyo,Minako Heima,Raymond Luo,Richard T. Haasch,Jake I. Gold,Miho Yamauchi,Paul J. A. Kenis,Paul J. A. Kenis +8 more
TL;DR: Based on surface valence band spectra, geometric effects rather than electronic effects seem to be key in determining the selectivity of bimetallic Cu-Pd catalysts, which implies that selectivities to different products can be tuned by geometric arrangements.
Journal ArticleDOI
Theoretical insights into a CO dimerization mechanism in CO2 electroreduction
TL;DR: DFT simulations that demonstrate the ability of Cu to catalyze CO dimerization in CO2 and CO electroreduction with cations other than H(+) are presented, a finding that is consistent with the experimentally observed pH independence of C2 formation on Cu.
Journal ArticleDOI
Achieving Highly Efficient, Selective, and Stable CO2 Reduction on Nitrogen-Doped Carbon Nanotubes.
Jingjie Wu,Ram Manohar Yadav,Mingjie Liu,Pranav P. Sharma,Chandra Sekhar Tiwary,Lulu Ma,Xiaolong Zou,Xiao-Dong Zhou,Boris I. Yakobson,Jun Lou,Pulickel M. Ajayan +10 more
TL;DR: It is reported that carbon nanotubes, doped with nitrogen to form resident electron-rich defects, can act as highly efficient and, more importantly, stable catalysts for the conversion of CO2 to CO.
Journal ArticleDOI
Electrochemical Activation of CO2 through Atomic Ordering Transformations of AuCu Nanoparticles
Dohyung Kim,Chenlu Xie,Nigel Becknell,Yi Yu,Mohammadreza Karamad,Mohammadreza Karamad,Karen Chan,Karen Chan,Ethan J. Crumlin,Jens K. Nørskov,Jens K. Nørskov,Peidong Yang +11 more
TL;DR: It is shown that the atomic ordering transformation, applied to AuCu NPs, activates them to perform as selective electrocatalysts for CO2 reduction, in contrast to the disordered alloy NP.
Journal ArticleDOI
A metal-free electrocatalyst for carbon dioxide reduction to multi-carbon hydrocarbons and oxygenates
Jingjie Wu,Sichao Ma,Jing Sun,Jake I. Gold,Chandra Sekhar Tiwary,Byoungsu Kim,Byoungsu Kim,Lingyang Zhu,Nitin Chopra,Ihab N. Odeh,Robert Vajtai,Aaron Z. Yu,Raymond Luo,Jun Lou,Guqiao Ding,Paul J. A. Kenis,Paul J. A. Kenis,Pulickel M. Ajayan +17 more
TL;DR: It is reported that nanometre-size N-doped graphene quantum dots (NGQDs) catalyse the electrochemical reduction of carbon dioxide into multi-carbon hydrocarbons and oxygenates at high Faradaic efficiencies, high current densities and low overpotentials.
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Progress and Perspectives of Electrochemical CO2 Reduction on Copper in Aqueous Electrolyte
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