Ethanol Dehydrogenation over Copper-Silica Catalysts: From Sub-Nanometer Clusters to 15 nm Large Particles

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dc.contributor.authorPokorný, Tomášcs
dc.contributor.authorVykoukal, Vítcs
dc.contributor.authorMacháč, Petrcs
dc.contributor.authorMoravec, Zdeněkcs
dc.contributor.authorScott, Nicholascs
dc.contributor.authorRoupcová, Pavlacs
dc.contributor.authorKarásková, Kateřinacs
dc.contributor.authorStyskalik, Alešcs
dc.coverage.issue30cs
dc.coverage.volume11cs
dc.date.issued2023-06-20cs
dc.description.abstractComparison of four preparation methodsshowed that the simpleand cost-effective dry impregnation provides Cu/SiO2 materialshowing the most stable catalytic behavior in potential renewableacetaldehyde production despite having a broad particle size distribution. Non-oxidative ethanoldehydrogenation is a renewable source ofacetaldehyde and hydrogen. The reaction is often catalyzed by supportedcopper catalysts with high selectivity. The activity and long-termstability depend on many factors, including particle size, choiceof support, doping, etc. Herein, we present four different syntheticpathways to prepare Cu/SiO2 catalysts (& SIM;2.5 wt %Cu) with varying copper distribution: hydrolytic sol-gel (sub-nanometerclusters), dry impregnation (A = 3.4 nm; & sigma;= 0.9 nm and particles up to 32 nm), strong electrostatic adsorption(A = 3.1 nm; & sigma; = 0.6 nm), and solvothermalhot injection followed by Cu particle deposition (A = 4.0 nm; & sigma; = 0.8 nm). All materials were characterized byICP-OES, XPS, N-2 physisorption, STEM-EDS, XRD, RFC N2O, and H-2-TPR and tested in ethanol dehydrogenationfrom 185 to 325 & DEG;C. The sample prepared by hydrolytic sol-gelexhibited high Cu dispersion and, accordingly, the highest catalyticactivity. Its acetaldehyde productivity (2.79 g g(-1) h(-1) at 255 & DEG;C) outperforms most of the Cu-basedcatalysts reported in the literature, but it lacks stability and tendsto deactivate over time. On the other hand, the sample prepared bysimple and cost-effective dry impregnation, despite having Cu particlesof various sizes, was still highly active (2.42 g g(-1) h(-1) acetaldehyde at 255 & DEG;C). Importantly,it was the most stable sample out of the studied materials. The characterizationof the spent catalyst confirmed its exceptional properties: it showedthe lowest extent of both coking and particle sintering.en
dc.formattextcs
dc.format.extent10980-10992cs
dc.format.mimetypeapplication/pdfcs
dc.identifier.citationACS Sustainable Chemistry and Engineering. 2023, vol. 11, issue 30, p. 10980-10992.en
dc.identifier.doi10.1021/acssuschemeng.2c06777cs
dc.identifier.issn2168-0485cs
dc.identifier.orcid0000-0002-3969-5837cs
dc.identifier.other187313cs
dc.identifier.researcheridD-8788-2012cs
dc.identifier.scopus9436200300cs
dc.identifier.urihttp://hdl.handle.net/11012/244969
dc.language.isoencs
dc.publisherAmerican Chemical Societycs
dc.relation.ispartofACS Sustainable Chemistry and Engineeringcs
dc.relation.urihttps://pubs.acs.org/doi/10.1021/acssuschemeng.2c06777cs
dc.rightsCreative Commons Attribution 4.0 Internationalcs
dc.rights.accessopenAccesscs
dc.rights.sherpahttp://www.sherpa.ac.uk/romeo/issn/2168-0485/cs
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/cs
dc.subjectethanol dehydrogenationen
dc.subjectcopperen
dc.subjectnanoparticlesen
dc.subjectacetaldehydeen
dc.subjectsol-gelen
dc.subjectdry impregnationen
dc.titleEthanol Dehydrogenation over Copper-Silica Catalysts: From Sub-Nanometer Clusters to 15 nm Large Particlesen
dc.type.driverarticleen
dc.type.statusPeer-revieweden
dc.type.versionpublishedVersionen
sync.item.dbidVAV-187313en
sync.item.dbtypeVAVen
sync.item.insts2025.02.03 15:51:31en
sync.item.modts2025.01.17 16:35:01en
thesis.grantorVysoké učení technické v Brně. Středoevropský technologický institut VUT. Sdílená laboratoř RP1cs
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