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Palladium versus Platinum: The Metal in the Catalytic Center of a Molecular Photocatalyst Determines the Mechanism of the Hydrogen Production with Visible Light

Pfeffer, Michael G.; Schaefer, Bernhard; Smolentsev, Grigory LU ; Uhlig, Jens; Nazarenko, Elena; Guthmuller, Julien; Kuhnt, Christian; Waechtler, Maria; Dietzek, Benjamin and Sundström, Villy LU , et al. (2015) In Angewandte Chemie (International edition) 54(17). p.5044-5048
Abstract
To develop highly efficient molecular photocatalysts for visible light-driven hydrogen production, a thorough understanding of the photophysical and chemical processes in the photocatalyst is of vital importance. In this context, in situ X-ray absorption spectroscopic (XAS) investigations show that the nature of the catalytically active metal center in a (N boolean AND N)MCl2 (M=Pd or Pt) coordination sphere has a significant impact on the mechanism of the hydrogen formation. Pd as the catalytic center showed a substantially altered chemical environment and a formation of metal colloids during catalysis, whereas no changes of the coordination sphere were observed for Pt as catalytic center. The high stability of the Pt center was confirmed... (More)
To develop highly efficient molecular photocatalysts for visible light-driven hydrogen production, a thorough understanding of the photophysical and chemical processes in the photocatalyst is of vital importance. In this context, in situ X-ray absorption spectroscopic (XAS) investigations show that the nature of the catalytically active metal center in a (N boolean AND N)MCl2 (M=Pd or Pt) coordination sphere has a significant impact on the mechanism of the hydrogen formation. Pd as the catalytic center showed a substantially altered chemical environment and a formation of metal colloids during catalysis, whereas no changes of the coordination sphere were observed for Pt as catalytic center. The high stability of the Pt center was confirmed by chloride addition and mercury poisoning experiments. Thus, for Pt a fundamentally different catalytic mechanism without the involvement of colloids is confirmed. (Less)
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publication status
published
subject
keywords
hydrogen production, palladium, photocatalysis, platinum, X-ray, adsorption spectroscopy
in
Angewandte Chemie (International edition)
volume
54
issue
17
pages
5044 - 5048
publisher
John Wiley & Sons
external identifiers
  • wos:000354190800008
  • scopus:85027933833
ISSN
1521-3773
DOI
10.1002/anie.201409438
language
English
LU publication?
yes
id
88ee1d41-e125-42f9-bf25-a15885746a67 (old id 7432627)
date added to LUP
2015-06-25 10:08:19
date last changed
2017-11-12 03:41:28
@article{88ee1d41-e125-42f9-bf25-a15885746a67,
  abstract     = {To develop highly efficient molecular photocatalysts for visible light-driven hydrogen production, a thorough understanding of the photophysical and chemical processes in the photocatalyst is of vital importance. In this context, in situ X-ray absorption spectroscopic (XAS) investigations show that the nature of the catalytically active metal center in a (N boolean AND N)MCl2 (M=Pd or Pt) coordination sphere has a significant impact on the mechanism of the hydrogen formation. Pd as the catalytic center showed a substantially altered chemical environment and a formation of metal colloids during catalysis, whereas no changes of the coordination sphere were observed for Pt as catalytic center. The high stability of the Pt center was confirmed by chloride addition and mercury poisoning experiments. Thus, for Pt a fundamentally different catalytic mechanism without the involvement of colloids is confirmed.},
  author       = {Pfeffer, Michael G. and Schaefer, Bernhard and Smolentsev, Grigory and Uhlig, Jens and Nazarenko, Elena and Guthmuller, Julien and Kuhnt, Christian and Waechtler, Maria and Dietzek, Benjamin and Sundström, Villy and Rau, Sven},
  issn         = {1521-3773},
  keyword      = {hydrogen production,palladium,photocatalysis,platinum,X-ray,adsorption spectroscopy},
  language     = {eng},
  number       = {17},
  pages        = {5044--5048},
  publisher    = {John Wiley & Sons},
  series       = {Angewandte Chemie (International edition)},
  title        = {Palladium versus Platinum: The Metal in the Catalytic Center of a Molecular Photocatalyst Determines the Mechanism of the Hydrogen Production with Visible Light},
  url          = {http://dx.doi.org/10.1002/anie.201409438},
  volume       = {54},
  year         = {2015},
}