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@ARTICLE{Zhu:903865,
      author       = {Zhu, Xinwei and Huang, Jun and Eikerling, Michael},
      title        = {{E}lectrochemical {CO} 2 {R}eduction at {S}ilver from a
                      {L}ocal {P}erspective},
      journal      = {ACS catalysis},
      volume       = {11},
      number       = {23},
      issn         = {2155-5435},
      address      = {Washington, DC},
      publisher    = {ACS},
      reportid     = {FZJ-2021-05498},
      pages        = {14521 - 14532},
      year         = {2021},
      abstract     = {The electrochemical reduction of CO2 to chemical fuels and
                      value-added chemicals is a viable pathway to store renewably
                      generated electrical energy and to mitigate the negative
                      impact of anthropogenic CO2 production. Herein, we study how
                      the local reaction environment dictates the mechanism and
                      kinetics of CO2 reduction to CO at an Ag electrode. The
                      local reaction environment is determined using a
                      hierarchical model that accounts for multistep reaction
                      kinetics, specific surface charging state at a given
                      electrode potential, and mass transport phenomena. The model
                      reveals vital mechanistic insights into the reaction
                      behavior. The increasing Tafel slope with overpotential is
                      seen to be influenced by the surface charging relation and
                      mass transport effects. In addition, the decrease of the CO
                      current density at high overpotentials is found to be caused
                      not only by the decrease in CO2 concentration due to mass
                      transport, surface charge effects, and pH increase but also
                      by lateral interactions between HCOOad, COOHad, and Had.
                      Moreover, we explore how the electrolyte properties,
                      including bicarbonate concentration, solvated cation size,
                      and CO2 partial pressure, tune the local reaction
                      environment.},
      cin          = {IEK-13},
      ddc          = {540},
      cid          = {I:(DE-Juel1)IEK-13-20190226},
      pnm          = {1231 - Electrochemistry for Hydrogen (POF4-123)},
      pid          = {G:(DE-HGF)POF4-1231},
      typ          = {PUB:(DE-HGF)16},
      UT           = {WOS:000753063400022},
      doi          = {10.1021/acscatal.1c04791},
      url          = {https://juser.fz-juelich.de/record/903865},
}