Mostrar el registro sencillo del ítem
dc.contributor.author
Mayer, Sergio Federico
dc.contributor.author
Falcon, Horacio
dc.contributor.author
Fernández Díaz, María Teresa
dc.contributor.author
Campos Martín, Jose Miguel
dc.contributor.author
Alonso, José Antonio
dc.date.available
2021-10-28T20:12:44Z
dc.date.issued
2020-07-13
dc.identifier.citation
Mayer, Sergio Federico; Falcon, Horacio; Fernández Díaz, María Teresa; Campos Martín, Jose Miguel; Alonso, José Antonio; Structure-properties relationship in the hydronium-containing pyrochlores (H3O)1+: PSb1+ pTe1- pO6with catalytic activity in the fructose dehydration reaction; Royal Society of Chemistry; Dalton Transactions; 49; 33; 13-7-2020; 11657-11667
dc.identifier.issn
1477-9226
dc.identifier.uri
http://hdl.handle.net/11336/145406
dc.description.abstract
A series of defect pyrochlores of the composition (H3O)1+pSb1+pTe1−pO6 have been prepared by ion exchange from K-containing pyrochlores K1+pSb1+pTe1−pO6 in sulfuric acid at 280 °C for 24 h. The structural characterization of the hydronium-containing pyrochlores, including the location of the H3O+ units within the three-dimensional framework, was possible from neutron powder diffraction data in undeuterated samples. The crystal structure for all the compounds is defined in the Fd3¯m space group, and consists of a covalent framework of SbV O6 and TeVIO6 octahedra distributed at random and connected by their vertices with (Sb,Te)–O1–(Sb,Te) angles close to 136°, conforming to large cages where the hydronium species are located off-center. The absence of K+ ions in the ion-exchanged pyrochlores was confirmed by inductively coupled plasma optical emission spectroscopy and scanning electron microscopy coupled with energy dispersive X-ray spectroscopy. The shape and size of the hydronium units evolve along with the series, becoming more compact as the framework covalence and Lewis-basicity decrease upon Sb enrichment of the structure (for greater p values). The amount and lability of the H3O+ species also increase throughout the series, as wanted: a straightforward correlation of the catalytic activity in the fructose dehydration reaction to 5-hydroxymethylfurfural has been observed, reaching conversion rates up to 88.5% of concentrated fructose solution for the p = 0.25 catalyst. Moreover, a pseudofirst-order kinetic mechanism was simulated, and the kinetic constants obtained from diluted and concentrated enhanced reaction systems were determined and compared.
dc.format
application/pdf
dc.language.iso
eng
dc.publisher
Royal Society of Chemistry
dc.rights
info:eu-repo/semantics/restrictedAccess
dc.rights.uri
https://creativecommons.org/licenses/by-nc-sa/2.5/ar/
dc.subject
5-hydroxymethylfurfural
dc.subject
Neutron powder diffraction
dc.subject
Pyrochlore
dc.subject
Kinetic mechanism
dc.subject.classification
Ingeniería Química
dc.subject.classification
Ingeniería Química
dc.subject.classification
INGENIERÍAS Y TECNOLOGÍAS
dc.title
Structure-properties relationship in the hydronium-containing pyrochlores (H3O)1+: PSb1+ pTe1- pO6with catalytic activity in the fructose dehydration reaction
dc.type
info:eu-repo/semantics/article
dc.type
info:ar-repo/semantics/artículo
dc.type
info:eu-repo/semantics/publishedVersion
dc.date.updated
2021-10-18T15:45:58Z
dc.identifier.eissn
1477-9234
dc.journal.volume
49
dc.journal.number
33
dc.journal.pagination
11657-11667
dc.journal.pais
Reino Unido
dc.journal.ciudad
Cambridge
dc.description.fil
Fil: Mayer, Sergio Federico. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación en Nanociencia y Nanotecnología; Argentina. Instituto de Ciencia de Materiales de Madrid; España. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba; Argentina
dc.description.fil
Fil: Falcon, Horacio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Córdoba. Centro de Investigación y Tecnología Química. Universidad Tecnológica Nacional. Facultad Regional Córdoba. Centro de Investigación y Tecnología Química; Argentina
dc.description.fil
Fil: Fernández Díaz, María Teresa. Institut Laue Langevin; Francia
dc.description.fil
Fil: Campos Martín, Jose Miguel. Consejo Superior de Investigaciones Científicas. Instituto de Catálisis y Petroleoquímica; España
dc.description.fil
Fil: Alonso, José Antonio. Instituto de Ciencia de Materiales de Madrid; España
dc.journal.title
Dalton Transactions
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/doi/https://doi.org/10.1039/D0DT01770A
dc.relation.alternativeid
info:eu-repo/semantics/altIdentifier/url/https://pubs.rsc.org/en/content/articlelanding/2020/dt/d0dt01770a/unauth
Archivos asociados