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dc.contributor.author | Rodríguez-Fernández, Aída | es_ES |
dc.contributor.author | Di Iorio, J. R. | es_ES |
dc.contributor.author | Paris Carrizo, Cecilia Gertrudis | es_ES |
dc.contributor.author | Boronat, Mercedes | es_ES |
dc.contributor.author | Corma, Avelino | es_ES |
dc.contributor.author | Román-Leshkov, Y. | es_ES |
dc.contributor.author | Moliner Marín, Manuel | es_ES |
dc.date.accessioned | 2021-03-12T16:30:06Z | - |
dc.date.available | 2021-03-12T16:30:06Z | - |
dc.date.issued | 2020-09-07 | - |
dc.identifier | issn: 2041-6539 | - |
dc.identifier.citation | Chemical Science 11: 10225- 10235 (2020) | es_ES |
dc.identifier.uri | http://hdl.handle.net/10261/234649 | - |
dc.description.abstract | The selective incorporation of isolated framework Lewis acid sites at specific crystallographic positions in high-silica zeolites was achieved by applying a rationalized post-synthetic grafting methodology. The removal of framework Ge atoms from a Ge-BEC zeolite with low concentrations of Ge in the framework (Si/Ge ∼ 150) followed by grafting allows the synthesis of Sn-BEC zeolites with Sn atoms positionally biased into the double-4-ring (D4R) crystallographic positions of the BEC framework. Spectroscopic characterization using solid-state nuclear magnetic resonance (NMR) coupled with theoretical calculations revealed that Sn atoms preferentially form open Sn sites in the D4R of Sn-BEC. This observation was supported by IR spectra of adsorbed deuterated acetonitrile (CD3CN), a known titrant of Sn sites in zeolites. The catalytic implications of selective incorporation of open Sn sites in Sn-BEC were probed using the Meerwein-Ponndorf-Verley-Oppenauer (MPVO) reaction. Although the MPVO turnover rates normalized by the total number of open Sn sites were comparable on Sn-BEC and a conventional Sn-Beta catalyst synthesized in fluoride media (Sn-Beta(F)), Sn-BEC demonstrated higher per gram reaction rates because of its larger fraction of open sites compared to Sn-Beta(F). These results highlight the advantage of placing active sites in targeted locations within a zeolite structure. The methodology presented here to selectively place catalytic active sites via sacrificial heteroatoms, such as Ge, can be generalized for the design of many other tetrahedrally-coordinated metal-containing zeolites. This journal is | - |
dc.description.sponsorship | This work has been supported by the Spanish Government-MINECO through ‘‘Severo Ochoa” (SEV-2016-0683), MAT2017-82288-C2-1-P (AEI/FEDER, UE) and RTI2018-101033-B-I00 (MCIU/AEI/FEDER, UE), and by Generalitat Valenciana through AICO/2019/060. JRD and YR-L thank the U.S. Department of Energy, Office of Basic Energy Sciences under Award No. DE-SC0016214 for support. ARF acknowledges the Spanish Government-MINECO for a FPU scholarship (FPU2017/01521). The Electron Microscopy Service of the UPV is acknowledged for their help in sample characterization. | - |
dc.language | eng | - |
dc.publisher | Royal Society of Chemistry (UK) | es_ES |
dc.relation | info:eu-repo/grantAgreement/MINECO/Plan Estatal de Investigación Científica y Técnica y de Innovación 2013-2016/SEV-2016-0683 | - |
dc.relation | info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/MAT2017-82288-C2-1-P | - |
dc.relation | info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/RTI2018-101033-B-I00 | - |
dc.relation.isversionof | Publisher's version | - |
dc.rights | openAccess | - |
dc.title | Selective active site placement in Lewis acid zeolites and implications for catalysis of oxygenated compounds | es_ES |
dc.type | artículo | es_ES |
dc.relation.publisherversion | http://dx.doi.org/10.1039/d0sc03809a | - |
dc.date.updated | 2021-03-12T16:30:07Z | - |
dc.rights.license | https://creativecommons.org/licenses/by-nc/3.0/ | - |
dc.contributor.funder | Ministerio de Economía, Industria y Competitividad (España) | - |
dc.contributor.funder | Generalitat Valenciana | - |
dc.contributor.funder | Ministerio de Ciencia, Innovación y Universidades (España) | - |
dc.relation.csic | Sí | es_ES |
dc.identifier.funder | http://dx.doi.org/10.13039/501100010198 | es_ES |
dc.identifier.funder | http://dx.doi.org/10.13039/501100003359 | es_ES |
dc.type.coar | http://purl.org/coar/resource_type/c_6501 | es_ES |
item.openairetype | artículo | - |
item.fulltext | With Fulltext | - |
item.openairecristype | http://purl.org/coar/resource_type/c_18cf | - |
item.cerifentitytype | Publications | - |
item.grantfulltext | open | - |
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