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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Published in | Angewandte Chemie (International ed.) Vol. 53; no. 47; pp. 12718 - 12722 |
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Main Authors | , , , , , , |
Format | Journal Article |
Language | English |
Published |
Weinheim
WILEY-VCH Verlag
17.11.2014
WILEY‐VCH Verlag Wiley Subscription Services, Inc |
Edition | International ed. in English |
Subjects | |
Online Access | Get full text |
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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.
The surface properties of supported metal hydrogenation catalysts are modified by the formation of microenvironments inside the catalyst pores and surrounding the metal nanoparticles. These microenvironments are derived from poly(vinyl alcohol) (PVA), and they are used to mitigate catalyst deactivation that is due to biogenic impurities. |
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Bibliography: | ArticleID:ANIE201407615 National Science Foundation - No. DGE-1256259 This material is based upon work supported by the National Science Foundation (EEC-0813570). We acknowledge Ana C. Alba-Rubio for collecting STEM images, and acknowledge the use of facilities and instrumentation supported by the University of Wisconsin Materials Research Science and Engineering Center (DMR-1121288). T.J.S. acknowledges support from the National Science Foundation Graduate Research Fellowship Program (DGE-1256259). Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the National Science Foundation. istex:55565DDB960EA70A6A952723A25A246F6A2048DC University of Wisconsin Materials Research Science and Engineering Center - No. DMR-1121288 National Science Foundation - No. EEC-0813570 ark:/67375/WNG-Z8KPXZZM-T This material is based upon work supported by the National Science Foundation (EEC‐0813570). We acknowledge Ana C. Alba‐Rubio for collecting STEM images, and acknowledge the use of facilities and instrumentation supported by the University of Wisconsin Materials Research Science and Engineering Center (DMR‐1121288). T.J.S. acknowledges support from the National Science Foundation Graduate Research Fellowship Program (DGE‐1256259). Any opinions, findings, and conclusions or recommendations expressed in this material are those of the authors and do not necessarily reflect the views of the National Science Foundation. ObjectType-Article-1 SourceType-Scholarly Journals-1 ObjectType-Feature-2 content type line 23 |
ISSN: | 1433-7851 1521-3773 |
DOI: | 10.1002/anie.201407615 |