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http://hdl.handle.net/10261/21286
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dc.contributor.author | Zicovich-Wilson, Claudio M. | - |
dc.contributor.author | Gándara Barragán, Felipe | - |
dc.contributor.author | Monge, M. Ángeles | - |
dc.contributor.author | Camblor, Miguel Ángel | - |
dc.date.issued | 2010-02-18T09:37:30Z | - |
dc.identifier.citation | Journal of the American Chemical Society 132 (10): 3461–3471 (2010) | - |
dc.identifier.uri | 10261/21286 | - |
dc.description.abstract | Under specific synthesis conditions the crystallization of a dense silica zeolite (TON) is followed by its in situ transformation into a less dense and, in the absence of occluded species, less stable zeolite (ITW). Periodic ab initio calculations including energy corrections for van der Waals interactions as well as zero-point and thermal effects are used first to assess the relative stability of both SiO2 (calcined) phases and then to investigate host−guest interactions in the as-made zeolites, as well as their relative stability. The less dense SiO2-ITW is less stable than SiO2-TON, with an energy difference that is significantly larger than expected from their difference in molar volume. This extra destabilization is ascribed to the strained double 4-ring units of silica tetrahedra (D4R). Regarding the as-made materials, the organic cation fills in more efficiently the zeolitic voids in ITW than in TON, bringing about a larger stabilization in the former owing to the extension of the long-range addition of dispersion force contributions. On the other hand, fluoride induces a polarization of the silica framework that is highly localized in TON (showing pentacoordinated [SiO4/2F]− units) but has a large global character in ITW (where fluoride is encapsulated into D4R units). We argue that the structure-directing role toward D4R materials that has been proposed for fluoride consists fundamentally in the ability to induce a global polarization of the silica framework that allows relaxation of the strain associated with these units. In this sense, fluoride stabilizes the otherwise strained D4R-SiO2 frameworks making them reachable for crystallization. This work documents a case in which the structure directing agents “choose” a structure not kinetically but through stabilization. | en_US |
dc.description.sponsorship | CICYT: MAT200603356 ConsoliderIngenio: CSD200600015 CONACYT: SEP0546983 FOMES2000 Project “Cómputo Científico" | en_US |
dc.language.iso | eng | en_US |
dc.publisher | American Chemical Society | - |
dc.rights | openAccess | en_US |
dc.source | Journal of the American Chemical Society | en_US |
dc.subject | Zeolites | en_US |
dc.subject | SiO2 | en_US |
dc.subject | Structure-direction | en_US |
dc.subject | synthesis | en_US |
dc.subject | Stability | en_US |
dc.subject | In situ transformation | en_US |
dc.subject | periodic calculations | en_US |
dc.subject | dispersion corrected density functional | en_US |
dc.title | In Situ Transformation of TON Silica Zeolite into the Less Dense ITW: Structure-Direction Overcoming Framework Instability in the Synthesis of SiO2 Zeolites | en_US |
dc.type | artículo | en_US |
dc.identifier.doi | 10.1021/ja9094318 | - |
dc.description.peerreviewed | Peer reviewed | en_US |
dc.relation.publisherversion | http://pubs.acs.org/articlesonrequest/AOR-fNrRnvBZV7t8GxZzZQeA | en_US |
dc.type.coar | http://purl.org/coar/resource_type/c_6501 | es_ES |
item.openairetype | artículo | - |
item.grantfulltext | open | - |
item.cerifentitytype | Publications | - |
item.openairecristype | http://purl.org/coar/resource_type/c_18cf | - |
item.fulltext | With Fulltext | - |
item.languageiso639-1 | en | - |
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Tontitw_revczwmac final.pdf | 472,6 kB | Adobe PDF | Visualizar/Abrir | |
Graphabasfinal2.tif | 54,09 kB | TIFF | Visualizar/Abrir |
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