Kinetic model for Pd-based membranes coking/deactivation in propane dehydrogenation processes

dc.contributor.authorBrencio, Camilla
dc.contributor.authorGough, Robin
dc.contributor.authorde Leeuw den Bouter, Anouk
dc.contributor.authorArratibel, Alba
dc.contributor.authorDi Felice, Luca
dc.contributor.authorGallucci, Fausto
dc.contributor.institutionTECNOLOGÍA DE MEMBRANAS E INTENSIFICACIÓN DE PROCESOS
dc.date.issued2023-01-15
dc.descriptionPublisher Copyright: © 2022 The Author(s)
dc.description.abstractThis work aims at providing insight into the deactivation mechanism of Pd-based membranes in propane dehydrogenation processes. Thermogravimetric analysis (TGA) experiments were conducted to study the adsorption and coking of propylene over conventional thin layer (TL) and double-skinned (DS) Pd-based membranes under several operating conditions. A mechanistic monolayer-multilayer coke growth model was selected to mathematically describe the membrane coking observed during TGA experiments. In addition, the reaction rate of coke formation and its influence on membranes deactivation has been studied. The deactivation model able to describe the hydrogen flux decay over time suggests that monolayer coke is the main responsible for the membrane deactivation. Multilayer coke also causes deactivation but with a smaller order than monolayer coke, for both the TL and the DS membranes. Among the two membrane types, DS membrane deactivates faster, i.e. with a higher order than the TL membrane, which is equal to 1.55 for the former and 0.51 for the latter. This is related to the higher number of active sites available in the controlling step of the deactivation reaction, which are most probably given by the addition of the ceramic Al2O3 protective layer. XPS spectra further confirms that, in the presence of Pd, Al2O3 sites contribute to carbon formation by evidencing a different nature of carbon formed on the two membranes. Finally, the experimental results of hydrogen permeation over time conducted on different membranes types and operative conditions confirmed the validity of the derived and parametrized kinetic models for coke formation and membrane deactivation. The experimental findings and the kinetic model derived in this work provide essential tools for the design and optimization of membrane reactors for dehydrogenation processes.en
dc.description.statusPeer reviewed
dc.format.extent1
dc.format.extent2491620
dc.identifier.citationBrencio , C , Gough , R , de Leeuw den Bouter , A , Arratibel , A , Di Felice , L & Gallucci , F 2023 , ' Kinetic model for Pd-based membranes coking/deactivation in propane dehydrogenation processes ' , Chemical Engineering Journal , vol. 452 part 1 , 139125 , pp. 139125 . https://doi.org/10.1016/j.cej.2022.139125
dc.identifier.doi10.1016/j.cej.2022.139125
dc.identifier.issn1385-8947
dc.identifier.otherresearchoutputwizard: 11556/1411
dc.identifier.urlhttp://www.scopus.com/inward/record.url?scp=85137770731&partnerID=8YFLogxK
dc.language.isoeng
dc.relation.ispartofChemical Engineering Journal
dc.rightsinfo:eu-repo/semantics/openAccess
dc.subject.keywordsMembrane deactivation
dc.subject.keywordsPropane dehydrogenation
dc.subject.keywordsHydrogen permeation
dc.subject.keywordsPd membranes
dc.subject.keywordsMembrane deactivation
dc.subject.keywordsPropane dehydrogenation
dc.subject.keywordsHydrogen permeation
dc.subject.keywordsPd membranes
dc.subject.keywordsGeneral Chemistry
dc.subject.keywordsEnvironmental Chemistry
dc.subject.keywordsGeneral Chemical Engineering
dc.subject.keywordsIndustrial and Manufacturing Engineering
dc.subject.keywordsProject ID
dc.subject.keywordsinfo:eu-repo/grantAgreement/EC/H2020/814671/EU/Bifunctional Zeolite based Catalysts and Innovative process for Sustainable Hydrocarbon Transformation/BIZEOLCAT
dc.subject.keywordsinfo:eu-repo/grantAgreement/EC/H2020/814671/EU/Bifunctional Zeolite based Catalysts and Innovative process for Sustainable Hydrocarbon Transformation/BIZEOLCAT
dc.subject.keywordsFunding Info
dc.subject.keywordsThis project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 814671 (BiZeolCat).
dc.subject.keywordsThis project has received funding from the European Union’s Horizon 2020 research and innovation program under grant agreement No 814671 (BiZeolCat).
dc.titleKinetic model for Pd-based membranes coking/deactivation in propane dehydrogenation processesen
dc.typejournal article
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