Identification of Sulfur-Tolerant Bimetallic Surfaces Using {DFT} Parametrized Models and Atomistic Thermodynamics

@article{kitchingroup-29,
  author =       {Inoglu, Nilay and Kitchin, John R.},
  title =        {Identification of Sulfur-Tolerant Bimetallic Surfaces Using
                  {DFT} Parametrized Models and Atomistic Thermodynamics},
  journal =      {ACS Catalysis},
  pages =        {399--407},
  year =         2011,
  doi =          {10.1021/cs200039t},
  abstract =     {The identification of sulfur-tolerant alloys for catalytic
                  applications is difficult due to the combinatorially large
                  number of alloy compositions and surface structures that may
                  be considered. Density functional theory calculations (DFT)
                  are not fast enough to enumerate all the possible structures
                  and their sulfur tolerance. In this work, a DFT parametrized
                  algebraic model that accounts for structure and composition
                  was used to estimate the d-band properties and sulfur
                  adsorption energies of 370 transition metal-based bimetallic
                  alloy surfaces.  The estimated properties were validated by
                  DFT calculations for 110 of the surface structures. We then
                  utilized an atomistic thermodynamic framework that includes
                  surface segregation, the presence of adsorbates, and effects
                  of environmental conditions to identify alloy compositions and
                  structures with enhanced sulfur tolerance that are likely to
                  be stable under the environmental conditions. As a case study,
                  we show how this database can be used to identify
                  sulfur-tolerant Cu-based catalysts and compare the results
                  with what is known about these catalysts experimentally.},
  issn =         {null},
  type =         {Journal Article},
}