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dc.contributor.authorDurndell, Lee
dc.contributor.authorIsaacs, MA
dc.contributor.authorLI, C
dc.contributor.authorParlett, C
dc.contributor.authorWilson, K
dc.contributor.authorLee, AF
dc.date.accessioned2019-04-30T10:47:54Z
dc.date.available2019-04-30T10:47:54Z
dc.date.issued2019-06-07
dc.identifier.issn2155-5435
dc.identifier.issn2155-5435
dc.identifier.otheracscatal.9b00092
dc.identifier.urihttp://hdl.handle.net/10026.1/13752
dc.description.abstract

Cascade reactions represent an atom-economical and energy-efficient technology by which to reduce the number of manipulations required for chemical manufacturing. Biocatalytic cascades are ubiquitous in nature; however, controlling the sequence of interactions between reactant, intermediate(s), and active sites remains a challenge for chemocatalysis. Here, we demonstrate an approach to achieve efficient cascades using chemical catalysts through flow chemistry. Close-coupling of Pd/SBA-15 and Pt/SBA-15 heterogeneous catalysts in a dual bed configuration under continuous flow operation affords a high single pass yield of 84% (a 20-fold enhancement over batch operation) and high stability for >14000 turnovers in the cascade oxidation of cinnamyl alcohol to cinnamic acid, despite both catalysts being individually inactive for this reaction. Judicious ordering of Pd (first bed) and Pt (second bed) catalysts is critical to promote cascade oxidation with respect to undesired hydrogenation and hydrogenolysis, the latter favored over the reverse-bed sequence or a single mixed PdPt reactor bed. The intrinsic catalytic performance of each bed is preserved in the optimal dual-bed configuration, enabling quantitative prediction of final product yields for reactants/intermediates whose individual oxidation behavior is established. Continuous processing using contiguous reactor beds enables plug-and-play design of cascades employing "simple" catalysts.

dc.format.extent5345-5352
dc.languageen
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)
dc.subjectcascade
dc.subjectflow chemistry
dc.subjectoxidation
dc.subjectpalladium
dc.subjectplatinum
dc.subjectalcohol
dc.titleCascade aerobic selective oxidation over contiguous dual catalyst beds in continuous flow
dc.typejournal-article
dc.typeJournal Article
plymouth.author-urlhttps://www.webofscience.com/api/gateway?GWVersion=2&SrcApp=PARTNER_APP&SrcAuth=LinksAMR&KeyUT=WOS:000471212600062&DestLinkType=FullRecord&DestApp=ALL_WOS&UsrCustomerID=11bb513d99f797142bcfeffcc58ea008
plymouth.issue6
plymouth.volume9
plymouth.publication-statusPublished
plymouth.journalACS Catalysis
dc.identifier.doi10.1021/acscatal.9b00092
plymouth.organisational-group/Plymouth
plymouth.organisational-group/Plymouth/Faculty of Science and Engineering
plymouth.organisational-group/Plymouth/Faculty of Science and Engineering/School of Geography, Earth and Environmental Sciences
plymouth.organisational-group/Plymouth/REF 2021 Researchers by UoA
plymouth.organisational-group/Plymouth/REF 2021 Researchers by UoA/UoA12 Engineering
plymouth.organisational-group/Plymouth/Users by role
plymouth.organisational-group/Plymouth/Users by role/Academics
dcterms.dateAccepted2019-04-29
dc.rights.embargodate2020-4-28
dc.identifier.eissn2155-5435
dc.rights.embargoperiodNot known
rioxxterms.versionofrecord10.1021/acscatal.9b00092
rioxxterms.licenseref.urihttp://www.rioxx.net/licenses/all-rights-reserved
rioxxterms.typeJournal Article/Review


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