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@ARTICLE{Schalenbach:1020444,
      author       = {Schalenbach, Maximilian and Raijmakers, Luc and Selmert,
                      Victor and Kretzschmar, Ansgar and Durmus, Yasin Emre and
                      Tempel, Hermann and Eichel, Rüdiger-A.},
      title        = {{H}ow {M}icrostructures, {O}xide {L}ayers, and {C}harge
                      {T}ransfer {R}eactions influence {D}ouble {L}ayer
                      {C}apacitances},
      journal      = {Physical chemistry, chemical physics},
      volume       = {26},
      number       = {19},
      issn         = {1463-9076},
      address      = {Cambridge},
      publisher    = {RSC Publ.},
      reportid     = {FZJ-2024-00164},
      pages        = {14288-14304},
      year         = {2024},
      abstract     = {Varying the electrode potential rearranges the charges in
                      the double layer (DL) of an electrochemical interface by a
                      resistive-capacitive current response. The capacitances of
                      such charge relocations are frequently used in the research
                      community to estimate electrochemical active surface areas
                      (ECSAs), yet the reliability of this methodology is
                      insufficiently examined. Here, the relation of capacitances
                      and ECSAs is critically assessed with electrochemical
                      impedance spectroscopy (EIS) and cyclic voltammetry (CV)
                      data on polished (Au, Ti, Ru, Pt, Ni, glassy carbon,
                      graphite plate) and porous (carbon fleeces) electrodes. By
                      investigating this variety of electrodes, the
                      frequency-dependencies observed in the measured capacitances
                      are shown to arise from the inherent resistive-capacitive DL
                      response, charge transfer reactions, and resistively damped
                      capacitive currents in microstructures (such as pores,
                      pinholes, or cracks). These frequency-dependencies are
                      typically overlooked when capacitances are related to ECSAs.
                      The capacitance at the specimen-characteristic relaxation
                      frequency of the resistive-capacitive DL response is
                      proposed as a standardized capacitance-metric to estimate
                      ECSAs. In 1 M perchloric acid, the polished gold electrode
                      and the high-surface area carbon fleeces show ratios of
                      capacitance-metric over surface-area of around 3.7 µF/cm².
                      Resistively damped currents in microstructures and
                      low-conducting oxide layers are shown to complicate
                      trustworthy capacitance-based estimations of ECSAs. In the
                      second part of this study, advanced equivalent circuits
                      models to describe the measured EIS and CV responses are
                      presented.},
      cin          = {IEK-9},
      ddc          = {540},
      cid          = {I:(DE-Juel1)IEK-9-20110218},
      pnm          = {1232 - Power-based Fuels and Chemicals (POF4-123)},
      pid          = {G:(DE-HGF)POF4-1232},
      typ          = {PUB:(DE-HGF)16},
      pubmed       = {38693897},
      UT           = {WOS:001216696500001},
      doi          = {10.1039/D3CP04743A},
      url          = {https://juser.fz-juelich.de/record/1020444},
}