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Title: Effect of nanostructured carbon support on copper electrocatalytic activity toward CO 2 electroreduction to hydrocarbon fuels

The effect of support on electrocatalytic activity of Cu nanoparticles (NPs) towards CO 2 electroreduction to hydrocarbon fuels (CH 4 and C 2H 4) is investigated for three types of nanostructured carbons: single wall carbon nanotubes (SWNT), graphene (GP) and onion-like carbon (OLC). Cu/SWNT, Cu/GP and Cu/OLC composite catalysts are synthesized and characterized by X-Ray diffraction analysis, transmission electron microscopy and electrochemical surface area measurements. Electrocatalytic activities of the synthesized materials, as measured in an electrochemical cell connected to a gas chromatograph, are compared to that of Cu NPs supported on Vulcan carbon. All four catalysts demonstrate higher activity towards C 2H 4 generation vs CH 4, with production of the latter mostly suppressed on Cu NPs supported on nanostructured substrates. Onset potentials for C 2H 4 vs CH 4 generation are shifted positively by 200 mV for Cu/SWNT, Cu/GP, and Cu/OLC catalysts. The Cu/OLC catalyst is found to be superior to the other two nanostructured catalysts in terms of stability, activity and selectivity towards C 2H 4 generation. Its faradaic efficiency reached 60% at -1.8 V vs Ag/AgCl. The enhanced activity and stability of Cu/OLC catalyst can be attributed to the unique catalyst design, wherein a shell of OLCmore » surrounds the Cu NPs such that the outer layer acts as a filter that protects the Cu surface from adsorption of undesirable species, enhances its electrocatalytic performance, and improves its viability in CO 2 electroreduction reaction.« less
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [1] ;  [1] ;  [1] ;  [1] ;  [3]
  1. Naval Research Lab. (NRL), Washington, DC (United States)
  2. Univ. of Oxford (United Kingdom)
  3. Drexel Univ., Philadelphia, PA (United States)
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 288; Journal Issue: C; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1394472

Baturina, Olga, Lu, Qin, Xu, Feng, Purdy, Andrew, Dyatkin, Boris, Sang, Xiahan, Unocic, Raymond, Brintlinger, Todd, and Gogotsi, Yury. Effect of nanostructured carbon support on copper electrocatalytic activity toward CO2 electroreduction to hydrocarbon fuels. United States: N. p., Web. doi:10.1016/j.cattod.2016.11.001.
Baturina, Olga, Lu, Qin, Xu, Feng, Purdy, Andrew, Dyatkin, Boris, Sang, Xiahan, Unocic, Raymond, Brintlinger, Todd, & Gogotsi, Yury. Effect of nanostructured carbon support on copper electrocatalytic activity toward CO2 electroreduction to hydrocarbon fuels. United States. doi:10.1016/j.cattod.2016.11.001.
Baturina, Olga, Lu, Qin, Xu, Feng, Purdy, Andrew, Dyatkin, Boris, Sang, Xiahan, Unocic, Raymond, Brintlinger, Todd, and Gogotsi, Yury. 2016. "Effect of nanostructured carbon support on copper electrocatalytic activity toward CO2 electroreduction to hydrocarbon fuels". United States. doi:10.1016/j.cattod.2016.11.001. https://www.osti.gov/servlets/purl/1394472.
@article{osti_1394472,
title = {Effect of nanostructured carbon support on copper electrocatalytic activity toward CO2 electroreduction to hydrocarbon fuels},
author = {Baturina, Olga and Lu, Qin and Xu, Feng and Purdy, Andrew and Dyatkin, Boris and Sang, Xiahan and Unocic, Raymond and Brintlinger, Todd and Gogotsi, Yury},
abstractNote = {The effect of support on electrocatalytic activity of Cu nanoparticles (NPs) towards CO2 electroreduction to hydrocarbon fuels (CH4 and C2H4) is investigated for three types of nanostructured carbons: single wall carbon nanotubes (SWNT), graphene (GP) and onion-like carbon (OLC). Cu/SWNT, Cu/GP and Cu/OLC composite catalysts are synthesized and characterized by X-Ray diffraction analysis, transmission electron microscopy and electrochemical surface area measurements. Electrocatalytic activities of the synthesized materials, as measured in an electrochemical cell connected to a gas chromatograph, are compared to that of Cu NPs supported on Vulcan carbon. All four catalysts demonstrate higher activity towards C2H4 generation vs CH4, with production of the latter mostly suppressed on Cu NPs supported on nanostructured substrates. Onset potentials for C2H4 vs CH4 generation are shifted positively by 200 mV for Cu/SWNT, Cu/GP, and Cu/OLC catalysts. The Cu/OLC catalyst is found to be superior to the other two nanostructured catalysts in terms of stability, activity and selectivity towards C2H4 generation. Its faradaic efficiency reached 60% at -1.8 V vs Ag/AgCl. The enhanced activity and stability of Cu/OLC catalyst can be attributed to the unique catalyst design, wherein a shell of OLC surrounds the Cu NPs such that the outer layer acts as a filter that protects the Cu surface from adsorption of undesirable species, enhances its electrocatalytic performance, and improves its viability in CO2 electroreduction reaction.},
doi = {10.1016/j.cattod.2016.11.001},
journal = {Catalysis Today},
number = C,
volume = 288,
place = {United States},
year = {2016},
month = {11}
}