Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Improved CO2 reduction activity towards C2+ alcohols on a tandem gold on copper electrocatalyst

Journal Article · · Nature Catalysis

Here, the discovery of materials for the electrochemical transformation of carbon dioxide into liquid fuels has the potential to impact large-scale storage of renewable energies and reduce carbon emissions. Here, we report the discovery of an electrocatalyst composed of gold nanoparticles on a polycrystalline copper foil (Au/Cu) that is highly active for CO2 reduction to alcohols. At low overpotentials, the Au/Cu electrocatalyst is over 100 times more selective for the formation of products containing C–C bonds versus methane or methanol, largely favouring the generation of alcohols over hydrocarbons. A combination of electrochemical testing and transport modelling supports the hypothesis that CO2 reduction on gold generates a high CO concentration on nearby copper, where CO is further reduced to alcohols such as ethanol and n-propanol under locally alkaline conditions. The bimetallic Au/Cu electrocatalyst exhibits synergistic activity and selectivity superior to gold, copper or AuCu alloys, and opens new possibilities for the development of CO2 reduction electrodes exploiting tandem catalysis mechanisms.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1490634
Journal Information:
Nature Catalysis, Journal Name: Nature Catalysis Journal Issue: 10 Vol. 1; ISSN 2520-1158
Publisher:
Springer NatureCopyright Statement
Country of Publication:
United States
Language:
English

References (55)

Spectroscopic Observation of a Hydrogenated CO Dimer Intermediate During CO Reduction on Cu(100) Electrodes journal February 2017
Stability of Residual Oxides in Oxide‐Derived Copper Catalysts for Electrochemical CO 2 Reduction Investigated with 18 O Labeling journal December 2017
Spectroscopic Observation of a Hydrogenated CO Dimer Intermediate During CO Reduction on Cu(100) Electrodes journal February 2017
Stability of Residual Oxides in Oxide-Derived Copper Catalysts for Electrochemical CO 2 Reduction Investigated with 18 O Labeling journal December 2017
Insights into CC Coupling in CO 2 Electroreduction on Copper Electrodes journal January 2013
Effects of Anion Identity and Concentration on Electrochemical Reduction of CO 2 journal February 2018
Electrocatalytic Alloys for CO 2 Reduction journal December 2017
High-Selectivity Electrochemical Conversion of CO 2 to Ethanol using a Copper Nanoparticle/N-Doped Graphene Electrode journal September 2016
Electrochemical CO2 Reduction on Metal Electrodes book January 2008
Calculation for the cathode surface concentrations in the electrochemical reduction of CO2 in KHCO3 solutions journal October 2005
Electrochemical evidence of intermediate formation of adsorbed CO in cathodic reduction of CO2 at a nickel electrode journal November 1990
In situ AFM observations of oxide film formation o n Cu(111) and Cu (100) surfaces under aqueous alkaline solutions journal January 1995
Size-dependent reactivity of gold-copper bimetallic nanoparticles during CO2 electroreduction journal June 2017
The influence of pH on the reduction of CO and CO 2 to hydrocarbons on copper electrodes journal March 2014
Enhanced selectivity for the electrochemical reduction of CO2 to alcohols in aqueous solution with nanostructured Cu–Au alloy as catalyst journal April 2014
Electrochemical Reduction of Carbon Dioxide to Ethane Using Nanostructured Cu 2 O-Derived Copper Catalyst and Palladium(II) Chloride journal November 2015
Identification of Possible Pathways for C–C Bond Formation during Electrochemical Reduction of CO 2 : New Theoretical Insights from an Improved Electrochemical Model journal April 2016
Subsurface Oxygen in Oxide-Derived Copper Electrocatalysts for Carbon Dioxide Reduction journal December 2016
Nickel–Gallium-Catalyzed Electrochemical Reduction of CO 2 to Highly Reduced Products at Low Overpotentials journal February 2016
Tuning the Selectivity of Carbon Dioxide Electroreduction toward Ethanol on Oxide-Derived Cu x Zn Catalysts journal November 2016
Nanoporous Copper Films by Additive-Controlled Electrodeposition: CO 2 Reduction Catalysis journal April 2017
Experimental Parameters Influencing Hydrocarbon Selectivity during the Electrochemical Conversion of CO 2 journal November 2017
pH Effects on the Selectivity of the Electrocatalytic CO 2 Reduction on Graphene-Embedded Fe–N–C Motifs: Bridging Concepts between Molecular Homogeneous and Solid-State Heterogeneous Catalysis journal March 2018
Catalysis Research of Relevance to Carbon Management:  Progress, Challenges, and Opportunities journal April 2001
Catalyzing the Hydrogen Evolution Reaction (HER) with Molybdenum Sulfide Nanomaterials journal October 2014
Dendritic Assembly of Gold Nanoparticles during Fuel-Forming Electrocatalysis journal May 2014
Electrocatalytic Conversion of Carbon Dioxide to Methane and Methanol on Transition Metal Surfaces journal August 2014
Probing the Active Surface Sites for CO Reduction on Oxide-Derived Copper Electrocatalysts journal July 2015
Formation, Migration, and Reactivity of Au–CO Complexes on Gold Surfaces journal January 2016
Electrochemical Activation of CO 2 through Atomic Ordering Transformations of AuCu Nanoparticles journal June 2017
Promoter Effects of Alkali Metal Cations on the Electrochemical Reduction of Carbon Dioxide journal August 2017
Electrochemical CO 2 Reduction over Compressively Strained CuAg Surface Alloys with Enhanced Multi-Carbon Oxygenate Selectivity journal October 2017
Nanoporous Copper–Silver Alloys by Additive-Controlled Electrodeposition for the Selective Electroreduction of CO 2 to Ethylene and Ethanol journal April 2018
Temperature-Dependent Morphology Evolution and Surface Plasmon Absorption of Ultrathin Gold Island Films journal April 2012
CO 2 Electroreduction on Well-Defined Bimetallic Surfaces: Cu Overlayers on Pt(111) and Pt(211) journal September 2013
Electrochemical Reduction of CO at a Copper Electrode journal September 1997
Prospects of CO2 Utilization via Direct Heterogeneous Electrochemical Reduction journal December 2010
Activity Descriptors for CO 2 Electroreduction to Methane on Transition-Metal Catalysts journal January 2012
The Evolution of the Polycrystalline Copper Surface, First to Cu(111) and Then to Cu(100), at a Fixed CO 2 RR Potential: A Study by Operando EC-STM journal December 2014
Gold–Copper Nano-Alloy, “ Tumbaga ”, in the Era of Nano: Phase Diagram and Segregation journal October 2014
Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper journal April 2014
Highly selective plasma-activated copper catalysts for carbon dioxide reduction to ethylene journal June 2016
Understanding trends in electrochemical carbon dioxide reduction rates journal May 2017
A review of catalysts for the electroreduction of carbon dioxide to produce low-carbon fuels journal January 2014
Insights into the electrocatalytic reduction of CO 2 on metallic silver surfaces journal January 2014
Poisoning effect of adsorbed CO during CO 2 electroreduction on late transition metals journal January 2014
The effect of electrolyte composition on the electroreduction of CO 2 to CO on Ag based gas diffusion electrodes journal January 2016
Enhanced electrocatalytic activity of Au@Cu core@shell nanoparticles towards CO 2 reduction journal January 2015
Electrochemical CO 2 reduction on Au surfaces: mechanistic aspects regarding the formation of major and minor products journal January 2017
New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces journal January 2012
Engineering Cu surfaces for the electrocatalytic conversion of CO 2 : Controlling selectivity toward oxygenates and hydrocarbons journal May 2017
Extended x-ray-absorption fine-structure and near-edge-structure studies on evaporated small clusters of Au journal April 1985
Design of Alloy Electrocatalysts for CO[sub 2] Reduction journal January 1991
Electrochemical Reduction of CO 2 at Cu Nanocluster / (101̅0) ZnO Electrodes journal January 2013
Nickel and Iron Modified Copper Electrode for Electroreduction of CO 2 by In-situ Electrodeposition journal September 1989

Cited By (22)

Morphology-Graded Silicon Nanowire Arrays via Chemical Etching: Engineering Optical Properties at the Nanoscale and Macroscale journal March 2020
Operando Insight into the Correlation between the Structure and Composition of CuZn Nanoparticles and Their Selectivity for the Electrochemical CO 2 Reduction journal November 2019
Computational and experimental demonstrations of one-pot tandem catalysis for electrochemical carbon dioxide reduction to methane journal July 2019
Hydroxide promotes carbon dioxide electroreduction to ethanol on copper via tuning of adsorbed hydrogen journal December 2019
Emerging Carbon‐Based Heterogeneous Catalysts for Electrochemical Reduction of Carbon Dioxide into Value‐Added Chemicals journal December 2018
Electrochemical Real‐Time Mass Spectrometry (EC‐RTMS): Monitoring Electrochemical Reaction Products in Real Time journal April 2019
Electrochemical Real-Time Mass Spectrometry (EC-RTMS): Monitoring Electrochemical Reaction Products in Real Time journal April 2019
Electrochemical Carbon Dioxide Splitting journal February 2019
Insight into the Formation and Transfer Process of the First Intermediate of CO 2 Reduction over Ag‐Decorated Dendritic Cu journal October 2019
Hybrid Cu 0 and Cu x + as Atomic Interfaces Promote High‐Selectivity Conversion of CO 2 to C 2 H 5 OH at Low Potential journal March 2020
AuCu Alloy Nanoparticle Embedded Cu Submicrocone Arrays for Selective Conversion of CO 2 to Ethanol journal June 2019
Fabrication of Hollow CoP/TiO x Heterostructures for Enhanced Oxygen Evolution Reaction journal December 2019
Double layer charging driven carbon dioxide adsorption limits the rate of electrochemical carbon dioxide reduction on Gold journal January 2020
Mechanistic reaction pathways of enhanced ethylene yields during electroreduction of CO2–CO co-feeds on Cu and Cu-tandem electrocatalysts journal October 2019
Rational catalyst and electrolyte design for CO2 electroreduction towards multicarbon products journal March 2019
Cooperative CO2-to-ethanol conversion via enriched intermediates at molecule–metal catalyst interfaces journal December 2019
Sequential catalysis enables enhanced C–C coupling towards multi-carbon alkenes and alcohols in carbon dioxide reduction: a study on bifunctional Cu/Au electrocatalysts journal January 2019
Understanding cation effects in electrochemical CO 2 reduction journal January 2019
Selective electrochemical CO 2 conversion to multicarbon alcohols on highly efficient N-doped porous carbon-supported Cu catalysts journal January 2020
Regulating C–C coupling in thermocatalytic and electrocatalytic CO x conversion based on surface science journal January 2019
“Hot edges” in an inverse opal structure enable efficient CO 2 electrochemical reduction and sensitive in situ Raman characterization journal January 2019
Steering CO 2 electroreduction toward ethanol production by a surface-bound Ru polypyridyl carbene catalyst on N-doped porous carbon journal December 2019

Figures / Tables (5)


Similar Records

Bimetallic Electrocatalysts for CO2 Reduction
Journal Article · Fri Oct 26 00:00:00 EDT 2018 · Topics in Current Chemistry · OSTI ID:1712665

Carbon dioxide reduction to alcohols using perovskite-type electrocatalysts
Journal Article · Sun Feb 28 23:00:00 EST 1993 · Journal of the Electrochemical Society; (United States) · OSTI ID:6759371

Selective Electrocatalytic Reduction of CO2 into CO at Small, Thiol-Capped Au/Cu Nanoparticles
Journal Article · Thu Aug 09 00:00:00 EDT 2018 · Journal of Physical Chemistry. C · OSTI ID:1477176

Related Subjects