% IMPORTANT: The following is UTF-8 encoded.  This means that in the presence
% of non-ASCII characters, it will not work with BibTeX 0.99 or older.
% Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or
% “biber”.

@INPROCEEDINGS{Zhang:1021441,
      author       = {Zhang, Yufan and Binninger, Tobias and Huang, Jun and
                      Eikerling, Michael},
      title        = {{E}ntanglement of {E}lectronic {I}nteractions and
                      {D}ouble-{L}ayer {C}harging for {S}upported
                      {E}lectrocatalyst {N}anoparticles {R}evealed by
                      {D}ensity-{P}otential {F}unctional {T}heory},
      reportid     = {FZJ-2024-00737},
      year         = {2023},
      abstract     = {Metal nanoparticles (NPs) on solid substrates are widely
                      used as (electro)catalysts. Electron transfer between the
                      catalyst NP and support material can strongly influence the
                      catalytic activity, a phenomenon referred to as electronic
                      metal-support interactions (EMSI) [1]. In situ X-ray
                      absorption spectroscopy (XAS) provides a mean to probe the
                      charging of catalyst NPs [2,3]. However, several key
                      questions remained unclear, including the spatial
                      distribution of transferred electrons and their actual
                      impact on the NP’s catalytically active surface in contact
                      with the electrolyte [4]. In addition, the charging
                      characteristics of the electric double-layer (EDL) around
                      the NP are affected by support and neighboring NPs [5].
                      Therefore, computer simulations are required to reveal the
                      interrelation between electronic and double-layer effects,
                      which is crucial for improving the catalytic activity of
                      supported NPs.In this study, we use the recently developed
                      framework of density-potential functional theory (DPFT)
                      which combines orbital-free density functional theory and
                      modified Poisson-Boltzmann theory to address solid and
                      electrolyte phases simultaneously under constant potentials
                      [6]. Our approach considers electronic phenomena like
                      electron spillover, which is beyond the scope of traditional
                      double-layer models. We also study the EDL of
                      nanometer-scale particles, which is typically beyond the
                      capability of DFT calculations.The effects of NP size,
                      proximity, and support work function probed by in situ
                      spectroscopy have sparked some controversies. Our model
                      offers a rationale for these controversies by uncovering the
                      interplay of electronic interactions and double-layer
                      charging under constant potential conditions. Specifically,
                      local reaction conditions, such as the local electric field
                      and cation concentration, are regulated.Our model is
                      relevant to experimental groups as it assists in the
                      interpretation of in situ spectroscopy data regarding the
                      distribution and catalytic consequences of transferred
                      electrons. For the community of DFT-calculation-based
                      materials screening, our model helps identify relevant
                      descriptors for the catalytic properties of supported
                      catalyst systems.},
      month         = {Sep},
      date          = {2023-09-03},
      organization  = {Annual meeting of international
                       society of electrochemistry, Lyon
                       (France), 3 Sep 2023 - 8 Sep 2023},
      subtyp        = {Other},
      cin          = {IEK-13},
      cid          = {I:(DE-Juel1)IEK-13-20190226},
      pnm          = {1231 - Electrochemistry for Hydrogen (POF4-123)},
      pid          = {G:(DE-HGF)POF4-1231},
      typ          = {PUB:(DE-HGF)24},
      doi          = {10.34734/FZJ-2024-00737},
      url          = {https://juser.fz-juelich.de/record/1021441},
}