Effect of nanostructured carbon support on copper electrocatalytic activity toward CO2 electroreduction to hydrocarbon fuels

Baturina, Olga; Lu, Qin; Xu, Feng; Purdy, Andrew; Dyatkin, Boris; Sang, Xiahan; Unocic, Raymond; Brintlinger, Todd; Gogotsi, Yury

doi:10.1016/j.cattod.2016.11.001

Effect of nanostructured carbon support on copper electrocatalytic activity toward CO₂ electroreduction to hydrocarbon fuels

Journal Article · Wed Nov 09 23:00:00 EST 2016 · Catalysis Today

DOI:https://doi.org/10.1016/j.cattod.2016.11.001· OSTI ID:1394472

Baturina, Olga ^[1]; Lu, Qin ^[1]; Xu, Feng ^[2]; Purdy, Andrew ^[1]; Dyatkin, Boris ^[1]; Sang, Xiahan ^[1]; Unocic, Raymond ^[1]; Brintlinger, Todd ^[1]; Gogotsi, Yury ^[3]

Naval Research Lab. (NRL), Washington, DC (United States)
Univ. of Oxford (United Kingdom)
Drexel Univ., Philadelphia, PA (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Fluid Interface Reactions, Structures and Transport Center (FIRST)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1394472

Alternate ID(s):: OSTI ID: 1703692

Journal Information:: Catalysis Today, Journal Name: Catalysis Today Journal Issue: C Vol. 288; ISSN 0920-5861

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Small and Narrowly Distributed Copper Nanoparticles Supported on Carbon Prepared by Surface Organometallic Chemistry for Selective Hydrogenation and CO ₂ Electroconversion Processes Mavrokefalos, Christos K.; Kaeffer, Nicolas; Liu, Hsueh‐Ju ChemCatChem, Vol. 12, Issue 1 https://doi.org/10.1002/cctc.201901414	journal	October 2019
Electrochemically Inspired Copper(II) Complex on Disposable Graphite Pencil Electrode for Effective Simultaneous Detection of Hypoxanthine, Xanthine, and Uric Acid Odewunmi, Nurudeen A.; Kawde, Abdel-Nasser; Ibrahim, Mohamed Electroanalysis, Vol. 30, Issue 10 https://doi.org/10.1002/elan.201800397	journal	July 2018
Template‐Free Cu Electrodeposition to Prepare Cu–Micro‐Brush Electrodes for Electrochemical CO ₂ Reduction Gu, Yueyuan; Li, Jindong; Wang, Luyang ChemistrySelect, Vol. 4, Issue 37 https://doi.org/10.1002/slct.201903097	journal	October 2019
Current progress of metallic and carbon-based nanostructure catalysts towards the electrochemical reduction of CO ₂ Hou, Liang; Yan, Jingze; Takele, Leta Inorganic Chemistry Frontiers, Vol. 6, Issue 12 https://doi.org/10.1039/c9qi00484j	journal	January 2019
FeNC catalysts for CO ₂ electroreduction to CO: effect of nanostructured carbon supports Karapinar, Dilan; Tran, Ngoc-Huan; Giaume, Domitille Sustainable Energy & Fuels, Vol. 3, Issue 7 https://doi.org/10.1039/c9se00214f	journal	January 2019
Tuning the Products of CO ₂ Electroreduction on a Ni ₃ Ga Catalyst Using Carbon Solid Supports Paris, Aubrey R.; Chu, An T.; B. O'Brien, Conor Journal of The Electrochemical Society, Vol. 165, Issue 7 https://doi.org/10.1149/2.0791807jes	journal	January 2018

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