Details

Autor(en) / Beteiligte

• Calle-Vallejo, Federico
• Martínez, José I.
• García-Lastra, Juan M.
• Sautet, Philippe
• Loffreda, David

Titel

Fast Prediction of Adsorption Properties for Platinum Nanocatalysts with Generalized Coordination Numbers

Ist Teil von

• Angewandte Chemie (International ed.), 2014-08, Vol.53 (32), p.8316-8319

Auflage

International ed. in English

Ort / Verlag

Weinheim: WILEY-VCH Verlag

Erscheinungsjahr

2014

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Platinum is a prominent catalyst for a multiplicity of reactions because of its high activity and stability. As Pt nanoparticles are normally used to maximize catalyst utilization and to minimize catalyst loading, it is important to rationalize and predict catalytic activity trends in nanoparticles in simple terms, while being able to compare these trends with those of extended surfaces. The trends in the adsorption energies of small oxygen‐ and hydrogen‐containing adsorbates on Pt nanoparticles of various sizes and on extended surfaces were analyzed through DFT calculations by making use of the generalized coordination numbers of the surface sites. This simple and predictive descriptor links the geometric arrangement of a surface to its adsorption properties. It generates linear adsorption‐energy trends, captures finite‐size effects, and provides more accurate descriptions than d‐band centers and usual coordination numbers. Unlike electronic‐structure descriptors, which require knowledge of the densities of states, it is calculated manually. Finally, it was shown that an approximate equivalence exists between generalized coordination numbers and d‐band centers. The trends in the adsorption energies of oxygen‐ and hydrogen‐containing adsorbates on various platinum nanoparticles and extended surfaces are analyzed. By means of generalized coordination numbers, it is possible to unify the trends among dissimilar structures and sizes. Adsorption energies for terraces, edges, corners, and adatoms and finite‐size effects could be accurately described.