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  A unified view on heterogeneous and homogeneous catalysts through a combination of spectroscopy and quantum chemistry

Maganas, D., Trunschke, A., Schlögl, R., & Neese, F. (2016). A unified view on heterogeneous and homogeneous catalysts through a combination of spectroscopy and quantum chemistry. Faraday Discussions, 188, 181-197. doi:10.1039/C5FD00193E.

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 Creators:
Maganas, Dimitrios1, Author              
Trunschke, Annette2, Author              
Schlögl, Robert2, 3, Author              
Neese, Frank1, Author              
Affiliations:
1Research Department Neese, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023886              
2Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
3Research Department Schlögl, Max Planck Institute for Chemical Energy Conversion, Max Planck Society, ou_3023874              

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 Abstract: Identifying catalytically active structures or intermediates in homogeneous and heterogeneous catalysis is a formidable challenge. However, obtaining experimentally verified insight into the active species in heterogeneous catalysis is a tremendously challenging problem. Many highly advanced spectroscopic and microscopic methods have been developed to probe surfaces. In this discussion we employ a combination of spectroscopic methods to study two closely related systems from the heterogeneous (the silica-supported vanadium oxide VOx/SBA-15) and homogeneous (the complex K[VO(O2)Hheida]) domains. Spectroscopic measurements were conducted strictly in parallel for both systems and consisted of oxygen K-edge and vanadium L-edge X-ray absorption measurements in conjunction with resonance Raman spectroscopy. It is shown that the full information content of the spectra can be developed through advanced quantum chemical calculations that directly address the sought after structure–spectra relationships. To this end we employ the recently developed restricted open shell configuration interaction theory together with the time-dependent theory of electronic spectroscopy to calculate XAS and rR spectra respectively. The results of the study demonstrate that: (a) a combination of several spectroscopic techniques is of paramount importance in identifying signature structural motifs and (b) quantum chemistry is an extremely powerful guide in cross connecting theory and experiment as well as the homogeneous and heterogeneous catalysis fields. It is emphasized that the calculation of spectroscopic observables provides an excellent way for the critical experimental validation of theoretical results.

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Language(s): eng - English
 Dates: 2015-11-252016-01-042016-07-01
 Publication Status: Published in print
 Pages: 17
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1039/C5FD00193E
 Degree: -

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Title: Faraday Discussions
  Abbreviation : Faraday Discuss.
Source Genre: Journal
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Publ. Info: London : Royal Society of Chemistry
Pages: - Volume / Issue: 188 Sequence Number: - Start / End Page: 181 - 197 Identifier: ISSN: 1359-6640
CoNE: https://pure.mpg.de/cone/journals/resource/954925269326