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  Prospects of Heterogeneous Hydroformylation with Supported Single Atom Catalysts

Amsler, J., Sarma, B. B., Agostini, G., Prieto, G., Plessow, P. N., & Studt, F. (2020). Prospects of Heterogeneous Hydroformylation with Supported Single Atom Catalysts. Journal of the American Chemical Society, 142(11), 5087-5096. doi:10.1021/jacs.9b12171.

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 Creators:
Amsler, Jonas1, Author
Sarma, Bidyut B.2, Author              
Agostini, Giovanni3, Author
Prieto, Gonzalo4, 5, Author              
Plessow, Philipp N.1, Author
Studt, Felix1, 6, Author
Affiliations:
1Institute of Catalysis Research and Technology, Karlsruhe Institute of Technology, Hermann-von-Helmholtz Platz 1, 76344 Eggenstein-Leopoldshafen, Germany, ou_persistent22              
2Research Department Schüth, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_1445589              
3ALBA Synchrotron Light Source, Carrer de la Llum 2-26, 08290 Cerdanyola del Vallès, Barcelona, Spain, ou_persistent22              
4Research Group Prieto, Max-Planck-Institut für Kohlenforschung, Max Planck Society, ou_2243639              
5ITQ Instituto de Tecnologı́a Quı́mica, Universitat Politècnica de València-Consejo Superior de Investigaciones Científicas (UPV-CSIC), Av. Los Naranjos s/n, 46022 Valencia, Spain, ou_persistent22              
6Institute for Chemical Technology and Polymer Chemistry, Karlsruhe Institute of Technology, Kaiserstr. 12, 76131 Karlsruhe, Germany, ou_persistent22              

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 Abstract: The potential of oxide-supported rhodium single atom catalysts (SACs) for heterogeneous hydroformylation was investigated both theoretically and experimentally. Using high-level domain-based local-pair natural orbital coupled cluster singles doubles with perturbative triples contribution (DLPNO–CCSD(T)) calculations, both stability and catalytic activity were investigated for Rh single atoms on different oxide surfaces. Atomically dispersed, supported Rh catalysts were synthesized on MgO and CeO2. While the CeO2-supported rhodium catalyst is found to be highly active, this is not the case for MgO, most likely due to increased confinement, as determined by extended X-ray absorption fine structure spectroscopy (EXAFS), that diminishes the reactivity of Rh complexes on MgO. This agrees well with our computational investigation, where we find that rhodium carbonyl hydride complexes on flat oxide surfaces such as CeO2(111) have catalytic activities comparable to those of molecular complexes. For a step edge on a MgO(301) surface, however, calculations show a significantly reduced catalytic activity. At the same time, calculations predict that stronger adsorption at the higher coordinated adsorption site leads to a more stable catalyst. Keeping the balance between stability and activity appears to be the main challenge for oxide supported Rh hydroformylation catalysts. In addition to the chemical bonding between rhodium complex and support, the confinement experienced by the active site plays an important role for the catalytic activity.

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Language(s): eng - English
 Dates: 2019-11-112020-03-062020-03-18
 Publication Status: Published in print
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.9b12171
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Title: Journal of the American Chemical Society
  Other : JACS
  Abbreviation : J. Am. Chem. Soc.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 142 (11) Sequence Number: - Start / End Page: 5087 - 5096 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870