Host-Guest and Guest-Guest Interactions of P- And N-Containing Structure Directing Agents Entrapped inside MFI-Type Zeolite by Multinuclear NMR Spectroscopy
| Autor: | Jorge Simancas, Joaquin Martinez-Ortigosa, J. Alejandro Vidal-Moya, Philippe Gaveau, Fernando Rey, Teresa Blasco, Bruno Alonso |
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| Přispěvatelé: | Institut Charles Gerhardt Montpellier - Institut de Chimie Moléculaire et des Matériaux de Montpellier (ICGM ICMMM), Ecole Nationale Supérieure de Chimie de Montpellier (ENSCM)-Centre National de la Recherche Scientifique (CNRS)-Université de Montpellier (UM)-Université Montpellier 1 (UM1)-Université Montpellier 2 - Sciences et Techniques (UM2)-Institut de Chimie du CNRS (INC), Univ Politecnica Valencia Consejo Super Invest, Inst Tecnol Quim UPV CSIC, Valencia 46022, Spain |
| Rok vydání: | 2019 |
| Předmět: |
Ge
02 engineering and technology 010402 general chemistry Molecular sieve 01 natural sciences Crystals Solid-state NMR chemistry.chemical_compound 5-Coordinate Silicon [CHIM.ANAL]Chemical Sciences/Analytical chemistry Physical and Theoretical Chemistry Zeolite Tetraethylammonium Preferential location Nuclear magnetic resonance spectroscopy [CHIM.MATE]Chemical Sciences/Material chemistry 021001 nanoscience & nanotechnology Probe Organic structure directing agent Molecular-Sieves 0104 chemical sciences Surfaces Coatings and Films Electronic Optical and Magnetic Materials Crystallography General Energy chemistry Solid-state nuclear magnetic resonance Zeolites sense organs ZSM-5 0210 nano-technology N-14 Solid-State NMR |
| Zdroj: | Digital.CSIC. Repositorio Institucional del CSIC instname Journal of Physical Chemistry C Journal of Physical Chemistry C, American Chemical Society, 2019, 123 (36), pp.22324-22334. ⟨10.1021/acs.jpcc.9b05689⟩ RiuNet. Repositorio Institucional de la Universitat Politécnica de Valéncia |
| ISSN: | 1932-7447 1932-7455 |
| DOI: | 10.1021/acs.jpcc.9b05689⟩ |
| Popis: | [EN] Highly crystalline pure silica MFI zeolites have been synthesized using tetraethylammonium (TEA), tetraethylphosphonium (TEP), or a mixture of both cations in different proportions as organic structure directing agents (OSDAs). The zeolites have been deeply characterized in order to get insight about the guest guest interactions involving the OSDAs and the guest host interactions involving the OSDAs and the inorganic framework, as well as the main features of the resulting materials. The results show that the average size of the MFI crystals decreases when TEP is present within the zeolite and that this cation is homogeneously distributed throughout the crystallites. The multinuclear NMR investigation (H-1, C-13, N-14, F-19, Si-29, P-31) indicates that TEP interacts with the zeolite host creating higher heterogeneity of the SiO4 crystallographic sites and a diminution on the mobility of fluorine atoms incorporated into the zeolite. Moreover, the presence of TEP influences the dynamics of the nitrogen atoms of the TEA molecules, and 2D heteronuclear correlation experiments give evidence on the spatial proximity of the TEA and TEP molecules in the MFI zeolites. Then, it is concluded that TEA and TEP are intimately mixed within the zeolite voids of the pure silica MFI samples synthesized by the dual template route. Financial support by the MINECO of Spain through the Severo Ochoa (SEV-2016-0683) and RTI2018-101784-B-I00 projects is gratefully acknowledged. The authors also thank the Microscopy Service of the Universitat Politecnica de Valencia for its assistance in microscopy characterization (FESEM equipment preparation). J.M.-O. (SEV-2012-0267-02) is grateful to the Severo Ochoa Program for a predoctoral fellowship. |
| Databáze: | OpenAIRE |
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