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Acidity and accessibility studies of desilicated ZSM-5 zeolites in terms of their effectiveness as catalysts in acid-catalyzed cracking processes

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Acidity and accessibility studies of desilicated ZSM-5 zeolites in terms of their effectiveness as catalysts in acid-catalyzed cracking processes

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dc.contributor.author Tarach, Karolina A. es_ES
dc.contributor.author Góra-Marek, Kinga es_ES
dc.contributor.author Martínez-Triguero, Joaquín es_ES
dc.contributor.author Melian-Cabrera, Ignacio es_ES
dc.date.accessioned 2020-11-04T04:31:57Z
dc.date.available 2020-11-04T04:31:57Z
dc.date.issued 2017-02-21 es_ES
dc.identifier.issn 2044-4753 es_ES
dc.identifier.uri http://hdl.handle.net/10251/154023
dc.description.abstract [EN] The structural, textural and acidic characteristics of hierarchical ZSM-5 (Si/Al = 18¿32), obtained with two desilication approaches, and the effect of these treatments on the reactivity in various cracking reactions of variable feedstock size and severity have been investigated. Emphasis is given to understanding the accessibility of acid sites; this was investigated by textural analysis, FTIR probe molecules (pyridine, trimethylacetonitrile and 2,4,6-trimethylpyridine) and reactions involving n-decane, 1,3,5-triisopropylbenzene (TIPB), and low and high-density polyethylene, LDPE and HDPE, respectively. Higher surface areas and a narrower pore size distribution were obtained for NaOH&TBAOH-treated materials, comparing to NaOH-treated ones. FTIR studies of pivalonitrile and collidine adsorption correlate well with the mesopore surface area. For n-decane cracking activity, the acid strength is a determining factor, revealing that the NaOH&TBAOH treatment gave stronger sites than NaOH, but lower than the native zeolite. In contrast, the TIPB cracking activity was improved by the developed mesoporosity of the alkaline treated zeolites, and this was correlated to the pivalonitrile and collidine accessibility factors. During the n-decane and TIPB cracking, hydrogen transfer reactions were reduced, leading to high olefin production for the NaOH&TBAOH materials due to the shorter microporous paths after desilication. The increased accessibility of the acid sites also leads to an enhanced cracking activity of polyethylenes at low conversions, as determined by a decrease in the T5% and T50%; both parameters are linearly dependent on the pivalonitrile and collidine accessibility factors, for LDPE and HDPE. The T5% for HDPE is more influenced by the accessibility factors than it is for the LDPE. This is interpreted to be the result of the branching degree of HDPE and LDPE; linear HDPE is more sensitive to the enhanced number of pore mouths of ZSM-5 channels on the mesopores. At high conversion, the influence on the T50% of the accessibility factors for HDPE and LDPE is weaker, suggesting that the cracking at this stage involves intermediate molecules of smaller size with fewer diffusional limitations. With respect to our own prior work, the chosen zeolite and the cracking of polyolefins gave more pronounced differences for the hierarchical ZSM-5. es_ES
dc.description.sponsorship K. T. thanks for financial support from the National Science Centre, Poland, Grant No. 2014/13/D/ST5/02761. I. M.-C. thanks De Nederlandse Organisatie voor Wetenschappelijk Onderzoek (NWO) for financial support, project no. 10284. K. G.-M. thanks for financial support from the National Science Centre, Poland, Grant No. 2015/18/E/ST4/00191. J.M.-T.thanks financial support from the Spanish Ministry of Economy and Competitiveness through the Severo Ochoa program (SEV-2012-0267) and the grant CTQ2015-68951-C3-1-R. M. J. Ortiz Iniesta is acknowledged for technical support in the TGA measurements. J. Datka is acknowledged for preliminary discussion on the results presented in the paper. es_ES
dc.language Inglés es_ES
dc.publisher The Royal Society of Chemistry es_ES
dc.relation.ispartof Catalysis Science & Technology es_ES
dc.rights Reserva de todos los derechos es_ES
dc.title Acidity and accessibility studies of desilicated ZSM-5 zeolites in terms of their effectiveness as catalysts in acid-catalyzed cracking processes es_ES
dc.type Artículo es_ES
dc.identifier.doi 10.1039/c6cy02609e es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//CTQ2012-37925-C03-01/ES/CATALIZADORES PARA LA ENERGIA Y EL MEDIOAMBIENTE: ACTIVACION SELECTIVA DE ENLACES S-H Y C-H/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/NWO//10284/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//CTQ2015-68951-C3-1-R/ES/TRATAMIENTOS CATALITICOS AVANZADOS PARA LA VALORIZACION DE LA BIOMASA Y LA ELIMINACION DE RESIDUOS ASOCIADOS/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/NCN//2014%2F13%2FD%2FST5%2F02761/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/NCN//2015%2F18%2FE%2FST4%2F00191/ es_ES
dc.relation.projectID info:eu-repo/grantAgreement/MINECO//SEV-2012-0267/ es_ES
dc.rights.accessRights Abierto es_ES
dc.contributor.affiliation Universitat Politècnica de València. Instituto Universitario Mixto de Tecnología Química - Institut Universitari Mixt de Tecnologia Química es_ES
dc.description.bibliographicCitation Tarach, KA.; Góra-Marek, K.; Martínez-Triguero, J.; Melian-Cabrera, I. (2017). Acidity and accessibility studies of desilicated ZSM-5 zeolites in terms of their effectiveness as catalysts in acid-catalyzed cracking processes. Catalysis Science & Technology. 7(4):858-873. https://doi.org/10.1039/c6cy02609e es_ES
dc.description.accrualMethod S es_ES
dc.relation.publisherversion https://doi.org/10.1039/c6cy02609e es_ES
dc.description.upvformatpinicio 858 es_ES
dc.description.upvformatpfin 873 es_ES
dc.type.version info:eu-repo/semantics/publishedVersion es_ES
dc.description.volume 7 es_ES
dc.description.issue 4 es_ES
dc.relation.pasarela S\355203 es_ES
dc.contributor.funder National Science Centre, Polonia es_ES
dc.contributor.funder Ministerio de Economía y Competitividad es_ES
dc.contributor.funder Netherlands Organization for Scientific Research es_ES
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