Engineering Catalyst Microenvironments for Metal-Catalyzed Hydrogenation of Biologically Derived Platform Chemicals

It is shown that microenvironments formed around catalytically active sites mitigate catalyst deactivation by biogenic impurities that are present during the production of biorenewable chemicals from biologically derived species. Palladium and ruthenium catalysts are inhibited by the presence of sul...

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Bibliographic Details
Published in:Angewandte Chemie 2014-11, Vol.126 (47), p.12932-12936
Main Authors: Schwartz, Thomas J., Johnson, Robert L., Cardenas, Javier, Okerlund, Adam, Da Silva, Nancy A., Schmidt-Rohr, Klaus, Dumesic, James A.
Format: Article
Language:English
Subjects:
Amino acids
Biomasse
Carbon
Catalysts
Chemistry
Deactivation
Decomposition reactions
Erneuerbare Chemikalien
Hydrierungen
Hydrogenation
Impurities
Katalysatorstabilität
Nanokomposite
Palladium
Sorbic acid
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Summary:It is shown that microenvironments formed around catalytically active sites mitigate catalyst deactivation by biogenic impurities that are present during the production of biorenewable chemicals from biologically derived species. Palladium and ruthenium catalysts are inhibited by the presence of sulfur‐containing amino acids; however, these supported metal catalysts are stabilized by overcoating with poly(vinyl alcohol) (PVA), which creates a microenvironment unfavorable for biogenic impurities. Moreover, deactivation of Pd catalysts by carbon deposition from the decomposition of highly reactive species is suppressed by the formation of bimetallic PdAu nanoparticles. Thus, a PVA‐overcoated PdAu catalyst was an order of magnitude more stable than a simple Pd catalyst in the hydrogenation of triacetic acid lactone, which is the first step in the production of biobased sorbic acid. A PVA‐overcoated Ru catalyst showed a similar improvement in stability during lactic acid hydrogenation to propylene glycol in the presence of methionine. Die Oberflächeneigenschaften von trägerfixierten metallbasierten Hydrierkatalysatoren können modifiziert werden, indem man Mikroumgebungen in den Katalysatorporen und um die Metall‐Nanopartikel erzeugt. Diese Mikroumgebungen sind von Polyvinylalkohol (PVA) abgeleitet und mildern die Katalysatordeaktivierung durch biogene Verunreinigungen.
ISSN:0044-8249
1521-3757
DOI:10.1002/ange.201407615