First-principles calculations of the atomic and electronic structure ofFcenters in the bulk and on the (001) surface ofSrTiO3

The atomic and electronic structure, formation energy, and the energy barriers for migration have been calculated for the neutral O vacancy point defect F center in cubic SrTiO3 employing various implementations of density functional theory DFT. Both bulk and TiO2-terminated 001 surface F centers have been considered. Supercells of different shapes containing up to 320 atoms have been employed. The limit of an isolated single oxygen vacancy in the bulk corresponds to a 270-atom supercell, in contrast to commonly used supercells containing 40– 80 atoms. Calculations carried out with the hybrid B3PW functional show that the F center level approaches the conduction band bottom to within 0.5 eV…

Maximum Noble-Metal Efficiency in Catalytic Materials: Atomically Dispersed Surface Platinum

International audience; Platinum is the most versatile element in catalysis, but it is rare and its high price limits large-scale applications, for example in fuel-cell technology. Still, conventional catalysts use only a small fraction of the Pt content, that is, those atoms located at the catalyst's surface. To maximize the noble-metal efficiency, the precious metal should be atomically dispersed and exclusively located within the outermost surface layer of the material. Such atomically dispersed Pt surface species can indeed be prepared with exceptionally high stability. Using DFT calculations we identify a specific structural element, a ceria ``nanopocket'', which binds Pt2+ so strongly…

Back Cover: Maximum Noble-Metal Efficiency in Catalytic Materials: Atomically Dispersed Surface Platinum (Angew. Chem. Int. Ed. 39/2014)

High efficiency of Pt2+ - CeO2 novel thin film catalyst as anode for proton exchange membrane fuel cells

Abstract The elevated price of Pt limits the large-scale implementation of commercial proton exchange membrane fuel cells, which effectively convert chemical energy into electricity. In order to increase the cost-efficiency in proton-exchange membrane fuel cells, we have designed a family of novel anode catalysts consisting of thin films of ceria with low Pt loadings sputtered on a nanostructured carbon support. Remarkably, only such small amounts of Pt are necessary for achieving power density values comparable to the reference commercial catalysts, which results in excellent specific activities of our samples. By combining photoelectron spectroscopy and catalytic performance analysis, we …

Rücktitelbild: Auf dem Weg zu größtmöglicher Effizienz bei der katalytischen Nutzung von Edelmetallen: atomar dispergiertes Oberflächen-Platin (Angew. Chem. 39/2014)

First principles simulations of F centers in cubic SrTiO 3

Atomic and electronic structure of regular and O-deficient SrTiO3 have been studied. Several types of first principles atomistic simulations: Hartree-Fock method, Density Functional Theory, and hybrid HF-DFT functionals, have been applied to periodic models that consider supercells of different sizes (ranging between 40 and 240 atoms). We confirm the ionic character of the Sr-O bonds and the high covalency of the Ti-O2 substructure. For the stoichiometric cubic crystal; the lattice constant and bulk modulus correctly reproduce the experimental data whereas the band gap is only properly obtained by the B3PW functional. The relaxed geometry around the F center shows a large expansion of the t…

Auf dem Weg zu größtmöglicher Effizienz bei der katalytischen Nutzung von Edelmetallen: atomar dispergiertes Oberflächen-Platin

Platin ist das am vielseitigsten eingesetzte Element in der Katalyse. Allerdings begrenzt der hohe Preis des Edelmetalls die Verwendung in vielen Bereichen, z. B. in Katalysatormaterialien fur Brennstoffzellen. Trotzdem nutzen konventionelle Katalysatoren oftmals nur einen Bruchteil ihres Pt-Gehaltes, namlich diejenigen Atome, die sich auf der Oberflache des Katalysators befinden. Eine effizientere Edelmetallnutzung setzt somit eine hohere, bevorzugt atomare Dispersion der Pt-Atome auf der Oberflache voraus. Tatsachlich ist es moglich, solche atomar dispergierten Pt-Spezies mit sehr hoher Stabilitat auf einer Katalysatoroberflache herzustellen. Mithilfe von DFT-Rechnungen identifizieren wir…