4.6 Article

Temperature-Dependent Structure and Electrochemical Behavior of RuO2/Carbon Nanocomposites

Journal

JOURNAL OF PHYSICAL CHEMISTRY C
Volume 115, Issue 39, Pages 19117-19128

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/jp206932w

Keywords

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Funding

  1. NSERC Canada
  2. NSERC
  3. CIHR
  4. University of Saskatchewan
  5. U.S. Department of Energy - Basic Energy Sciences
  6. University of Washington
  7. Simon Fraser University
  8. U.S. DOE [DE-AC02-06CH11357]
  9. Advanced Photon Source

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RuO2/carbon nanocomposites are promising materials for supercapacitor electrodes because of their high power and energy capabilities. Understanding their structural change against temperature and electrochemical potential is crucial for better supercapazitor performance of these nanocomposites. The present work involves the preparation of RuO2 nanoparticles in mesoporous carbon substrates using a consecutive impregnation method and subsequent annealing of the composites from 25 to 600 degrees C. X-ray diffraction (XRD), transmission electron microscopy (TEM), thermogravimetric analysis (TGA), Ru K- and L-edge X-ray absorption spectroscopy (XAS), ab initio calculations, cyclic voltammetry, and in situ electrochemical(XAS) are used to investigate the structural changes of RuO2 in the nanocomposite. The data show that the RuO2 transitions from a heavily hydrated to slightly hydrated form and then reduces to metallic Ru as temperature increases. The latter reduction of RuO2 occurs at much lower temperatures than those for bulk RuO2. Electrochemical analysis indicates that the specific capacitance of the nano-RuO2 in the nanocomposiie is significantly lower than that of bulk RuO2, implying that only a small amount of nanoRuO(2) present is electroactive. This finding coincides with the in situ electrochemical XAS study, in which nearly no change in the Ru K-edge XAS is observed for the nanocoraposite electrode under varied potentials, differing from the bulk RuO2. This work presents a comprehensive picture of the structural changes of RuO2/carbon nanocomposites against temperature and electrochemical potential.

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