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Cascade catalysis of highly active bimetallic Au/Pd nanoclusters: structure-function relationship investigation using anomalous small-angle X-ray scattering and UV-Vis spectroscopy

Haas, Sylvio LU ; Fenger, Robert ; Fertitta, Edoardo and Rademann, Klaus (2013) In Journal of Applied Crystallography 46. p.1353-1360
Abstract
Recently, a so-called 'crown-jewel' concept of preparation of Au/Pd-based colloidal nanoclusters has been reported [Zhang, Watanabe, Okumura, Haruta & Toshima (2011). Nat. Mater. 11, 49-52]. Here, a different way of preparing highly active Au/Pd-based nanoclusters is presented. The origin of the increased activity of Au/Pd-based colloidal bimetallic nanoclusters was unclear up to now. However, it is, in general, accepted that in the nanometre range (1-100 nm) the cluster size, shape and composition affect the structural characteristics (e. g. lattice symmetry, unit cell), electronic properties (e. g. band gap) and chemical properties (e. g. catalytic activity) of a material. Hence, a detailed study of the relationship between the... (More)
Recently, a so-called 'crown-jewel' concept of preparation of Au/Pd-based colloidal nanoclusters has been reported [Zhang, Watanabe, Okumura, Haruta & Toshima (2011). Nat. Mater. 11, 49-52]. Here, a different way of preparing highly active Au/Pd-based nanoclusters is presented. The origin of the increased activity of Au/Pd-based colloidal bimetallic nanoclusters was unclear up to now. However, it is, in general, accepted that in the nanometre range (1-100 nm) the cluster size, shape and composition affect the structural characteristics (e. g. lattice symmetry, unit cell), electronic properties (e. g. band gap) and chemical properties (e. g. catalytic activity) of a material. Hence, a detailed study of the relationship between the nanostructure of nanoclusters and their catalytic activity is presented here. The results indicate that a high surface-to-volume ratio of the nanoclusters combined with the presence of 'both' Au and Pd isolated regions at the surface are crucial to achieve a high catalytic activity. A detailed structure elucidation directly leads to a mechanistic proposal, which indeed explains the higher catalytic activity of Au/Pd-based catalysts compared with pure metallic Au or Pd. The mechanism is based on cascade catalysis induced by a single type of nanoparticle with an intermixed surface of Au and Pd. (Less)
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; ; and
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Journal of Applied Crystallography
volume
46
pages
1353 - 1360
publisher
International Union of Crystallography
external identifiers
  • wos:000324764500014
  • scopus:84884561798
ISSN
1600-5767
DOI
10.1107/S0021889813018190
language
English
LU publication?
yes
id
a1af645e-2337-42c1-bbd0-219e344822a9 (old id 4095895)
date added to LUP
2016-04-01 10:36:12
date last changed
2022-04-04 19:37:27
@article{a1af645e-2337-42c1-bbd0-219e344822a9,
  abstract     = {{Recently, a so-called 'crown-jewel' concept of preparation of Au/Pd-based colloidal nanoclusters has been reported [Zhang, Watanabe, Okumura, Haruta & Toshima (2011). Nat. Mater. 11, 49-52]. Here, a different way of preparing highly active Au/Pd-based nanoclusters is presented. The origin of the increased activity of Au/Pd-based colloidal bimetallic nanoclusters was unclear up to now. However, it is, in general, accepted that in the nanometre range (1-100 nm) the cluster size, shape and composition affect the structural characteristics (e. g. lattice symmetry, unit cell), electronic properties (e. g. band gap) and chemical properties (e. g. catalytic activity) of a material. Hence, a detailed study of the relationship between the nanostructure of nanoclusters and their catalytic activity is presented here. The results indicate that a high surface-to-volume ratio of the nanoclusters combined with the presence of 'both' Au and Pd isolated regions at the surface are crucial to achieve a high catalytic activity. A detailed structure elucidation directly leads to a mechanistic proposal, which indeed explains the higher catalytic activity of Au/Pd-based catalysts compared with pure metallic Au or Pd. The mechanism is based on cascade catalysis induced by a single type of nanoparticle with an intermixed surface of Au and Pd.}},
  author       = {{Haas, Sylvio and Fenger, Robert and Fertitta, Edoardo and Rademann, Klaus}},
  issn         = {{1600-5767}},
  language     = {{eng}},
  pages        = {{1353--1360}},
  publisher    = {{International Union of Crystallography}},
  series       = {{Journal of Applied Crystallography}},
  title        = {{Cascade catalysis of highly active bimetallic Au/Pd nanoclusters: structure-function relationship investigation using anomalous small-angle X-ray scattering and UV-Vis spectroscopy}},
  url          = {{http://dx.doi.org/10.1107/S0021889813018190}},
  doi          = {{10.1107/S0021889813018190}},
  volume       = {{46}},
  year         = {{2013}},
}