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
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
More filters
Journal ArticleDOI
The Importance of Cannizzaro-Type Reactions during Electrocatalytic Reduction of Carbon Dioxide
TL;DR: A seemingly catalytically inactive electrode, boron-doped diamond (BDD), is found to be active for CO2 and CO reduction to formaldehyde and even methane, and the results obtained here may explain the concomitant formation of acids and alcohols often observed during CO2 reduction.
Journal ArticleDOI
Nanomorphology-Enhanced Gas-Evolution Intensifies CO2 Reduction Electrochemistry
Thomas Burdyny,Percival J. Graham,Yuanjie Pang,Cao-Thang Dinh,Min Liu,Edward H. Sargent,David Sinton +6 more
TL;DR: In this article, the morphology of nanostructured electrodes enhances long-range CO2 transport via their influence on gas-evolution, leading to a 4-fold increase in the limiting current density compared to a nanoparticle-based catalyst alone.
Journal ArticleDOI
Surface reconstruction of pure-Cu single-crystal electrodes under CO-reduction potentials in alkaline solutions: A study by seriatim ECSTM-DEMS
Youn-Geun Kim,Alnald Javier,Jack H. Baricuatro,Daniel A. Torelli,Kyle D. Cummins,Chu F. Tsang,John C. Hemminger,Manuel P. Soriaga +7 more
TL;DR: In this article, the authors showed that a polycrystalline Cu electrode kept in 0.1 M KOH at − 0.9 V (SHE), a potential very close to that for electrochemical CO reduction, underwent a two-step surface reconstruction, initially to Cu(111, or Cu(pc)-[Cu(111)], and terminally to either Cu(100, or CoCoCoCo-CoCo)-Cu(100).
Journal ArticleDOI
Stability and Effects of Subsurface Oxygen in Oxide-Derived Cu Catalyst for CO2 Reduction
Chang Liu,Maicon Pierre Lourenço,Svante Hedström,Filippo Cavalca,Filippo Cavalca,Oscar Diaz-Morales,Hélio A. Duarte,Anders Nilsson,Lars G. M. Pettersson +8 more
TL;DR: In this article, a self-consistent charge density functional tight binding (SCC-DFTB) was used to stabilize the oxide-derived copper (OD-Cu) catalysts.
Journal ArticleDOI
Selective Electrochemical Reduction of CO2 to Ethylene on Nanopores-Modified Copper Electrodes in Aqueous Solution
Yuecheng Peng,Tian Wu,Libo Sun,Jean Marie Vianney Nsanzimana,Adrian C. Fisher,Xin Wang,Xin Wang +6 more
TL;DR: When used in electrolysis process, the as-prepared nanopores-modified electrodes can suppress the Faradaic efficiency toward methane to less than 1%, while keeping that of ethylene in a high level of 35% in aqueous 0.1 M KHCO3 solution under -1.3 V, thus revealing a remarkable selectivity toward ethylene production.
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