Adsorption of Carbon on Pd Clusters of Nanometer Size: A First-Principles Theoretical Study | Sciact - CRIS-system of Boreskov Institute of Catalysis

Adsorption of Carbon on Pd Clusters of Nanometer Size: A First-Principles Theoretical Study Full article

Journal

Journal of Chemical Physics
ISSN: 0021-9606 , E-ISSN: 1089-7690

Output data

Year: 2005, Volume: 122, Number: 17, Pages: 174705/1-174705/9 Pages count : 9 DOI: 10.1063/1.1888385

Tags

DENSITY-FUNCTIONAL THEORY; BOND-LENGTH; BASIS-SETS; ENERGY; CO; NANOPARTICLES; MOLECULES; ATOMS; APPROXIMATION; ENERGETICS

Authors

Neyman Konstantin M. ^1,2 , Inntam Chan ³ , Gordienko Alexei B. ⁴ , Yudanov Ilya V. ⁵ , Rösch Notker ³

Affiliations

1	Institució Catalana de Recerca i Estudis Avançats (ICREA), 08010 Barcelona, Spain
2	Departament de Química Física i Centre especial de Recerca en Química Teòrica, Universitat de Barcelona i Parc Cientific de Barcelona, 08028 Barcelona, Spain
3	Department Chemie, Technische Universität München, 85747 Garching, Germany
4	Department of Physics, Kemerovo State University, 650043 Kemerovo, Russia
5	Boreskov Institute of Catalysis, Russian Academy of Sciences, 630090 Novosibirsk, Russia

Funding (2)

1	German Research Foundation
2	Verband der Chemischen Industrie

Adsorbed atomic C species can be formed in the course of surface reactions and commonly decorate metal catalysts. We studied computationally C adsorption on Pd nanoclusters using an all-electron scalar relativistic density functional method. The metal particles under investigation, Pd55Pd55, Pd79Pd79, Pd85Pd85, Pd116Pd116, Pd140Pd140, and Pd146Pd146, were chosen as fragments of bulk Pd in the form of three-dimensional octahedral or cuboctahedral crystallites, exposing (111) and (100) facets as well as edge sites. These cluster models are shown to yield size-converged adsorption energies. We examined which surface sites of these clusters are preferentially occupied by adsorbed C. According to calculations, surface C atoms form strongly adsorbed carbide species (with adsorption energies of more than 600kJmol−1600kJmol−1) bearing a significant negative charge. Surface sites allowing high, fourfold coordination of carbon are overall favored. To avoid effects of adsorbate-adsorbate interaction in the cluster models for carbon species in the vicinity of cluster edges, we reduced the local symmetry of selected adsorption complexes on the nanoclusters by lowering the global symmetry of the nanocluster models from point group OhOh to D4hD4h. On (111) facets, threefold hollow sites in the center are energetically preferred; adsorbed C is calculated to be slightly less stable when displaced to the facet borders.

Neyman K.M. , Inntam C. , Gordienko A.B. , Yudanov I.V. , Rösch N.
Adsorption of Carbon on Pd Clusters of Nanometer Size: A First-Principles Theoretical Study
Journal of Chemical Physics. 2005. V.122. N17. P.174705/1-174705/9. DOI: 10.1063/1.1888385 WOS Scopus РИНЦ ANCAN OpenAlex

Submitted:	Oct 27, 2004
Accepted:	Feb 16, 2005
Published print:	May 1, 2005
Published online:	May 3, 2005

Web of science:	WOS:000229064600044
Scopus:	2-s2.0-18744363415
Elibrary:	13485777
Chemical Abstracts:	2005:444236
Chemical Abstracts (print):	143:139915
OpenAlex:	W1985061132

DB	Citing
Web of science	33
Scopus	34
Elibrary	35
OpenAlex	35