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Synthetic control of the defect structure and hierarchical extra-large-/small-pore microporosity in aluminosilicate zeolite SWY
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dc.contributor.author | Chitac, Ruxandra-Georgiana | |
dc.contributor.author | Zholobenko, Vladimir | |
dc.contributor.author | Fletcher, Robin | |
dc.contributor.author | Softley, Emma | |
dc.contributor.author | Bradley, Jonathan | |
dc.contributor.author | Mayoral, Alvaro | |
dc.contributor.author | Turrina, Alessandro | |
dc.contributor.author | Wright, Paul A. | |
dc.date.accessioned | 2023-09-27T15:30:06Z | |
dc.date.available | 2023-09-27T15:30:06Z | |
dc.date.issued | 2023-10-11 | |
dc.identifier | 293818339 | |
dc.identifier | a839889e-1644-41df-8159-1884a20b6534 | |
dc.identifier | 85173578832 | |
dc.identifier.citation | Chitac , R-G , Zholobenko , V , Fletcher , R , Softley , E , Bradley , J , Mayoral , A , Turrina , A & Wright , P A 2023 , ' Synthetic control of the defect structure and hierarchical extra-large-/small-pore microporosity in aluminosilicate zeolite SWY ' , Journal of the American Chemical Society , vol. 145 , no. 40 , pp. 22097–22114 . https://doi.org/10.1021/jacs.3c07873 | en |
dc.identifier.issn | 0002-7863 | |
dc.identifier.other | ORCID: /0000-0002-4243-9957/work/143336463 | |
dc.identifier.uri | https://hdl.handle.net/10023/28461 | |
dc.description | R.G.C. thanks the University of St. Andrews and Johnson Matthey for funding. P.A.W. thanks the Royal Society (Industrial Fellowship INF\R2\192052) for support. R.G.C. acknowledges the support of the EPSRC Light Element Analysis Facility grant EP/T019298/1 and the EPSRC Strategic Equipment Resource grant EP/R023751/1 for the use of the Jeol JSM-IT800 electron microscope at the University of St Andrews. A.M. acknowledges the Spanish Ministry of Science (RYC2018-024561-I) and the Gobierno of Aragon (Nanomidas group, code E13_23R). | en |
dc.description.abstract | The SWY-type aluminosilicate zeolite, STA-30, has been synthesized via different routes to understand its defect chemistry and solid acidity. The synthetic parameters varied were the gel aging, the Al source, and the organic structure directing agent. All syntheses give crystalline materials with similar Si/Al ratios (6–7) that are stable in the activated K,H-form and closely similar by powder X-ray diffraction. However, they exhibit major differences in the crystal morphology and in their intracrystalline porosity and silanol concentrations. The diDABCO-C82+ (1,1′-(octane-1,8-diyl)bis(1,4-diazabicyclo[2.2.2]octan)-1-ium)-templated STA-30 samples (but not those templated by bisquinuclidinium octane, diQuin-C82+) possess hierarchical microporosity, consisting of noncrystallographic extra-large micropores (13 Å) that connect with the characteristic swy and gme cages of the SWY structure. This results in pore volumes up to 30% greater than those measured in activated diQuin-C8_STA-30 as well as higher concentrations of silanols and fewer Brønsted acid sites (BASs). The hierarchical porosity is demonstrated by isopentane adsorption and the FTIR of adsorbed pyridine, which shows that up to 77% of the BASs are accessible (remarkable for a zeolite that has a small-pore crystal structure). A structural model of single can/d6r column vacancies is proposed for the extra-large micropores, which is revealed unambiguously by high-resolution scanning transmission electron microscopy. STA-30 can therefore be prepared as a hierarchically porous zeolite via direct synthesis. The additional noncrystallographic porosity and, subsequently, the amount of SiOHs in the zeolites can be enhanced or strongly reduced by the choice of crystallization conditions. | |
dc.format.extent | 8677765 | |
dc.language.iso | eng | |
dc.relation.ispartof | Journal of the American Chemical Society | en |
dc.subject | QD Chemistry | en |
dc.subject | DAS | en |
dc.subject.lcc | QD | en |
dc.title | Synthetic control of the defect structure and hierarchical extra-large-/small-pore microporosity in aluminosilicate zeolite SWY | en |
dc.type | Journal article | en |
dc.contributor.sponsor | EPSRC | en |
dc.contributor.sponsor | EPSRC | en |
dc.contributor.sponsor | The Royal Society | en |
dc.contributor.institution | University of St Andrews. School of Chemistry | en |
dc.contributor.institution | University of St Andrews. EaSTCHEM | en |
dc.identifier.doi | https://doi.org/10.1021/jacs.3c07873 | |
dc.description.status | Peer reviewed | en |
dc.identifier.url | https://europepmc.org/article/MED/37755328 | en |
dc.identifier.grantnumber | EP/R023751/1 | en |
dc.identifier.grantnumber | EP/T019298/1 | en |
dc.identifier.grantnumber | INF\R2\192052 | en |
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