skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Electroreduction of carbon monoxide over a copper nanocube catalyst: Surface structure and pH dependence on selectivity

Journal Article · · ChemCatChem
ORCiD logo [1];  [2];  [3]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis
  2. Opus 12 Incorporated, Berkeley CA (United States)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). SUNCAT Center for Interface Science and Catalysis; AlbaNova University Center, Stockholm Univ., Stockholm (Sweden), Dept. of Physics

The activity and selectivity for CO2/CO reduction over copper electrodes is strongly dependent on the local surface structure of the catalyst and the pH of the electrolyte. Here we investigate a unique, copper nanocube surface (CuCube) as a CO reduction electrode under neutral and basic pH, using online electrochemical mass spectroscopy (OLEMS) to determine the onset potentials and relative intensities of methane and ethylene production. To relate the unique selectivity to the surface structure, the CuCube surface reactivity is compared to polycrystalline copper and three single crystals under the same reaction conditions. Here, we find that the high selectivity for ethylene over the CuCube surface is most comparable to the Cu(100) surface, which has the cubic unit cell. However, the suppression of methane production over CuCube is unique to that particular surface. Basic pH is also shown to enhance ethylene selectivity on all surfaces, again with the CuCube surface being unique.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
FA9550-10-1-0572, AC02-76SF00515
OSTI ID:
1311816
Journal Information:
ChemCatChem, Vol. 8, Issue 6; ISSN 1867-3880
Publisher:
ChemPubSoc EuropeCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 65 works
Citation information provided by
Web of Science

References (23)

Anthropogenic Chemical Carbon Cycle for a Sustainable Future journal August 2011
Powering the planet: Chemical challenges in solar energy utilization journal October 2006
Electrochemical CO2 Reduction on Metal Electrodes book January 2008
Electrochemical reduction of carbon dioxide at various series of copper single crystal electrodes journal May 2003
Electrochemical Reduction of CO at a Copper Electrode journal September 1997
Formation of hydrocarbons in the electrochemical reduction of carbon dioxide at a copper electrode in aqueous solution
  • Hori, Yoshio; Murata, Akira; Takahashi, Ryutaro
  • Journal of the Chemical Society, Faraday Transactions 1: Physical Chemistry in Condensed Phases, Vol. 85, Issue 8 https://doi.org/10.1039/f19898502309
journal January 1989
Production of Methane and Ethylene in Electrochemical Reduction of Carbon Dioxide at Copper Electrode in Aqueous Hydrogencarbonate Solution journal June 1986
Activity Descriptors for CO 2 Electroreduction to Methane on Transition-Metal Catalysts journal January 2012
How copper catalyzes the electroreduction of carbon dioxide into hydrocarbon fuels journal January 2010
New insights into the electrochemical reduction of carbon dioxide on metallic copper surfaces journal January 2012
High Selectivity for Ethylene from Carbon Dioxide Reduction over Copper Nanocube Electrocatalysts journal February 2015
High Selectivity for Ethylene from Carbon Dioxide Reduction over Copper Nanocube Electrocatalysts journal February 2015
Electroreduction of carbon monoxide to liquid fuel on oxide-derived nanocrystalline copper journal April 2014
Stable and selective electrochemical reduction of carbon dioxide to ethylene on copper mesocrystals journal January 2015
The importance of surface morphology in controlling the selectivity of polycrystalline copper for CO2 electroreduction journal January 2012
Structure effects on the energetics of the electrochemical reduction of CO2 by copper surfaces journal August 2011
Manipulating the Hydrocarbon Selectivity of Copper Nanoparticles in CO 2 Electroreduction by Process Conditions journal December 2014
Controlling the selectivity of CO2 electroreduction on copper: The effect of the electrolyte concentration and the importance of the local pH journal February 2016
The influence of pH on the reduction of CO and CO 2 to hydrocarbons on copper electrodes journal March 2014
A new mechanism for the selectivity to C1 and C2 species in the electrochemical reduction of carbon dioxide on copper electrodes journal January 2011
Two Pathways for the Formation of Ethylene in CO Reduction on Single-Crystal Copper Electrodes journal June 2012
Theoretical Insights into a CO Dimerization Mechanism in CO 2 Electroreduction journal May 2015
On-line mass spectrometry system for measurements at single-crystal electrodes in hanging meniscus configuration journal August 2006

Cited By (16)

Solute Incorporation at Oxide–Oxide Interfaces Explains How Ternary Mixed‐Metal Oxide Nanocrystals Support Element‐Specific Anisotropic Growth journal January 2020
Highly Selective Production of Ethylene by the Electroreduction of Carbon Monoxide journal December 2019
Highly Selective Production of Ethylene by the Electroreduction of Carbon Monoxide journal December 2019
Understanding trends in electrochemical carbon dioxide reduction rates journal May 2017
Copper-on-nitride enhances the stable electrosynthesis of multi-carbon products from CO2 journal September 2018
pH effects on the electrochemical reduction of CO(2) towards C2 products on stepped copper journal January 2019
Computational and experimental demonstrations of one-pot tandem catalysis for electrochemical carbon dioxide reduction to methane journal July 2019
Electrochemically converting carbon monoxide to liquid fuels by directing selectivity with electrode surface area journal June 2019
Electrochemical processes on solid shaped nanoparticles with defined facets journal January 2018
A computational exploration of CO 2 reduction via CO dimerization on mixed-valence copper oxide surface journal January 2018
Zn-Doped Cu(100) facet with efficient catalytic ability for the CO 2 electroreduction to ethylene journal January 2019
New aspects of C2 selectivity in electrochemical CO 2 reduction over oxide-derived copper journal January 2020
Cu nanowire-catalyzed electrochemical reduction of CO or CO 2 journal January 2019
Selective reduction of CO to acetaldehyde with CuAg electrocatalysts journal January 2020
Solute Incorporation at Oxide–Oxide Interfaces Explains How Ternary Mixed-Metal Oxide Nanocrystals Support Element-Specific Anisotropic Growth text January 2020
Origin of the selective electroreduction of carbon dioxide to formate by chalcogen modified copper text January 2018