Formation of active sites on transition metals through reaction-driven migration of surface atoms

Adopting low-index single-crystal surfaces as models for metal nanoparticle catalysts has been questioned by the experimental findings of adsorbate-induced formation of subnanometer clusters on several single-crystal surfaces. We used density functional theory calculations to elucidate the conditions that lead to cluster formation and show how adatom formation energies enable efficient screening of the conditions required for adsorbate-induced cluster formation. We studied a combination of eight face-centered cubic transition metals and 18 common surface intermediates and identified systems relevant to catalytic reactions, such as carbon monoxide (CO) oxidation and ammonia (NH 3 ) oxidation. We used kinetic…

• UD
  U.S. Department of Energy

  Awards: -AC02-05CH11231, BES-ERCAP0022773, AC02-06CH11357, FG02-05ER15731, 05CH11231, AC02-05CH11231, DE-AC02, DE-FG02-05ER15731, 06CH11357, DE-FG02-, DE-AC02-05CH11231, DE-AC02-06CH11357, DE-FG02, DE-AC02-
• AC
  Adolph C. and Mary Sprague Miller Institute for Basic Research in Science, University of California Berkeley
• NE
  National Energy Research Scientific Computing Center

  Awards: 05CH11231, BES-ERCAP0022773, AC02-05CH11231
• DF
  Deutsche Forschungsgemeinschaft

  Awards: 390776260, DE-AC02-06CH11357, DE-AC02-05CH11231, EXC 2089/1, EXC 2089/1-390776260, EXC 2089, 2089/1-390776260
• BA
  Bayerische Akademie der Wissenschaften
• OO
  Office of Science

  Awards: DE-AC02-06CH11357, DE-FG02-05ER15731, AC02-05CH11231, -AC02-05CH11231, DE-AC02, 06CH11357, AC02-06CH11357
• BE
  Basic Energy Sciences

  Awards: DE-AC02, KC31SM, AC02-05CH11231, DE-AC02-05CH11231, DE-FG02, AC02-06CH11357, 06CH11357, -AC02-05CH11231, DE-FG02-05ER15731
• AN
  Argonne National Laboratory

  Awards: DE-AC02, DE-AC02-05CH11231, 06CH11357, AC02-06CH11357
• DO
  Division of Materials Sciences and Engineering

  Awards: DE-AC02, AC02-05CH11231, DE-AC02-06CH11357, DE-AC02-05CH11231