Towards stable single-atom catalysts: strong binding of atomically dispersed transition metals on the surface of nanostructured ceria

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DOI

  • Alberto Figueroba, Univ Barcelona, University of Barcelona, Inst Quim Teor & Computac IQTCUB
  • ,
  • Gabor Kovacs, Univ Barcelona, University of Barcelona, Inst Quim Teor & Computac IQTCUB
  • ,
  • Albert Bruix
  • ,
  • Konstantin M. Neyman, ICREA, Centre for Research in Agricultural Genomics (CRAG) and Facultat de Veterinaria UAB, Campus Universitat Autonoma Barcelona

The interaction of a series of different transition metal atoms with nanoparticulate CeO2 has been studied by means of density-functional calculations. Recently, we demonstrated the ability of sites exposed on {100} nanofacets of CeO2 to very strongly anchor atomic Pt, making the formed species exceptionally efficient single-atom anode catalysts for proton-exchange membrane fuel cells. Herein, we analyzed the capacity of these surface sites to accommodate all other group VIII-XI transition metal atoms M = Fe, Ru, Os, Co, Rh, Ir, Ni, Pd, Cu, Ag, and Au. The interaction of the M atoms with {100} nanofacets of ceria leads to oxidation of the former and such interaction is calculated to be stronger than the binding of the atoms in the corresponding metal nanoparticles. Comparing the stability of metal-metal and metal-oxide bonds allows one to establish which metals would more strongly resist agglomeration and hence allows the proposal of promising candidates for the design of single-atom catalysts. Indeed, the remarkable stability of these adsorption complexes (particularly for Pt, Pd, Ni, Fe, Co, and Os) strongly suggests that atomically dispersed transition metals anchored as cations on {100} facets of nanostructured ceria are stable against agglomeration into metal particles. Therefore, these sites appear to be of immediate relevance to the preparation of stable catalysts featuring the highest possible metal efficiency in nanocatalysis.

Original languageEnglish
JournalCatalysis Science & Technology
Volume6
Issue18
Pages (from-to)6806-6813
Number of pages8
ISSN2044-4753
DOIs
Publication statusPublished - 2016

    Research areas

  • DENSITY-FUNCTIONAL THEORY, TOTAL-ENERGY CALCULATIONS, WAVE BASIS-SET, OXIDATION-STATE, CO OXIDATION, ELECTRONIC-STRUCTURE, SUPPORT INTERACTIONS, CEO2 NANOPARTICLES, PLATINUM, WATER

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