Research ArticleELECTROCHEMISTRY

Highly efficient electrochemical reforming of CH4/CO2 in a solid oxide electrolyser

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Science Advances  30 Mar 2018:
Vol. 4, no. 3, eaar5100
DOI: 10.1126/sciadv.aar5100
  • Fig. 1 The schematic of electrochemical CO2/CH4 reforming process in an SOE to produce syngas; CO2 electrolysis is performed in the cathode, whereas electrochemical oxidation of CH4 is performed in the anode.
  • Fig. 2 XRD patterns and microstructure of samples.

    (A and B) XRD of the oxidized samples (A) and reduced samples (B), respectively. a.u., arbitrary units; PDF, powder diffraction file. (C) SEM image of the reduced LSCM-Ni0.5Cu0.5. (D) Transmission electron microscopy (TEM) microscopic results of the reduced LSCM-Ni0.5Cu0.5.

  • Fig. 3 The performance of CO2 adsorption and coking resistance.

    (A) In situ FTIR spectroscopy of CO2 for a series of samples at 800°C. (B) The most stable adsorption configurations of CO2 on the defected site of the (Ni-Cu)/LCO (001) system surface. (C) Carbon coking resistance of LSCM-Ni0.5Cu0.5 with a flow of 20% CH4/H2 at 800°C for 4 hours. (D) TS of carbon removal. The energies for removal of chemisorbed carbon species on Ni/LCO (001) are relative to the dissociation of hydrogen on the Ni/LCO (001) interface. Asterisk denotes an adsorbed species on the Ni/LCO (001) surface.

  • Fig. 4 The performances of CO2 electrolysis.

    (A) The I-V curves of the electrolysers based on different cathode materials for CO2 electrolysis at 800°C. (B) The short-term performances of CO2 electrolysis at different applied voltages. (C and D) CO production (C) and current efficiencies (D) with various cathode materials.

  • Fig. 5 The performances of the electrochemical reforming of CH4/CO2.

    (A) The I-V curves of the CO2 electrolysis with simultaneous electrochemical oxidation of CH4 electrolysers based on different anode materials at 800°C. (B) The short-term performances of the electrochemical reforming of CH4/CO2 at different applied voltages. (C) In situ ac impedance spectroscopy with different anodes at different applied voltages. Rp, polarization resistance. (D) CO production and H2 production in anode with various anode materials.

Supplementary Materials

  • Supplementary material for this article is available at http://advances.sciencemag.org/cgi/content/full/4/3/eaar5100/DC1

    fig. S1. XPS results of oxidized and reduced samples.

    fig. S2. Thermogravimetric analysis (TGA) of reduced samples and the conductivities of reduced samples.

    fig. S3. The best configurations for chemisorption of CO2 on system surface and corresponding differential charge density.

    fig. S4. Different configurations for chemisorption of CO2 on the M/LCO (001) system surface.

    fig. S5. The configurations for chemisorption of CO2 on the M/LCO (001) system defected surface and the corresponding molecular dynamics calculation.

    fig. S6. SEM image for the single cells.

    fig. S7. The ac impedance spectra of the electrolyzers.

    fig. S8. The ac impedance spectra of the electrolyzers for single solid oxide cells.

    fig. S9. The long-term and redox cycling performance of the symmetric cell.

    table S1. The adsorption energies, bond distances, and bond angle after CO2 adsorption and charge analysis of a partial system.

  • Supplementary Materials

    This PDF file includes:

    • fig. S1. XPS results of oxidized and reduced samples.
    • fig. S2. Thermogravimetric analysis (TGA) of reduced samples and the conductivities of reduced samples.
    • fig. S3. The best configurations for chemisorption of CO2 on system surface and corresponding differential charge density.
    • fig. S4. Different configurations for chemisorption of CO2 on the M/LCO (001) system surface.
    • fig. S5. The configurations for chemisorption of CO2 on the M/LCO (001) system defected surface and the corresponding molecular dynamics calculation.
    • fig. S6. SEM image for the single cells.
    • fig. S7. The ac impedance spectra of the electrolyzers.
    • fig. S8. The ac impedance spectra of the electrolyzers for single solid oxide cells.
    • fig. S9. The long-term and redox cycling performance of the symmetric cell.
    • table S1. The adsorption energies, bond distances, and bond angle after CO2 adsorption and charge analysis of a partial system.

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