A Multi-Nuclear MAS-NMR Study on the Structural Properties of Silicalite-1 Zeolite Synthesized Using N- and P-Based Organic Structure Directing Agents
The nature of organic structure directing agents (OSDAs) is of paramount importance in the final properties of zeolites, particularly the framework and porosity. Recently, the use of P-containing OSDAs has been employed for new zeolites, but there is little discussion compared to their analogues N-O...
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MDPI AG
2021-07-01
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| Online Access: | https://www.mdpi.com/2076-3417/11/15/6850 |
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| author | Joaquin Martinez-Ortigosa Jorge Simancas Jose A. Vidal-Moya Fernando Rey Susana Valencia Teresa Blasco |
| author_facet | Joaquin Martinez-Ortigosa Jorge Simancas Jose A. Vidal-Moya Fernando Rey Susana Valencia Teresa Blasco |
| author_sort | Joaquin Martinez-Ortigosa |
| collection | DOAJ |
| description | The nature of organic structure directing agents (OSDAs) is of paramount importance in the final properties of zeolites, particularly the framework and porosity. Recently, the use of P-containing OSDAs has been employed for new zeolites, but there is little discussion compared to their analogues N-OSDAs. The main objective of this work is the characterization of pure silica MFI zeolite (silicalite-1) prepared by the <i>dual-template</i> route with tetrapropylammonium (TPA), tetrapropylphosphonium (TPP) cations, and mixtures thereof aiming to understand by advanced NMR methods how the nature of the organic influences the physico-chemical properties of the zeolite. Silicalite-1 has been successfully synthesized using the <i>dual-template</i> procedure with TPA and TPP molecules. Both OSDAs are incorporated into the zeolite without any specific preference, differently to that observed before for the TEA/TEP system, and homogenously mixed inside of the zeolite voids. The presence of TPP leads to the incorporation of less F, raising the concentration of Q<sup>3</sup>-defective sites in the silicalite-1 zeolites. Detailed NMR results indicate that those structural defects are close to the –CH<sub>3</sub> group of the entrapped OSDAs in the zeolite and these defects consist of at least two silanol groups stabilizing the Si-O<sup>-</sup> species, which is responsible for the charge balancing. |
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| institution | Directory Open Access Journal |
| issn | 2076-3417 |
| language | English |
| last_indexed | 2024-03-10T09:18:48Z |
| publishDate | 2021-07-01 |
| publisher | MDPI AG |
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| series | Applied Sciences |
| spelling | doaj.art-62af41a062ae4fffb5850922131c6eea2023-11-22T05:20:40ZengMDPI AGApplied Sciences2076-34172021-07-011115685010.3390/app11156850A Multi-Nuclear MAS-NMR Study on the Structural Properties of Silicalite-1 Zeolite Synthesized Using N- and P-Based Organic Structure Directing AgentsJoaquin Martinez-Ortigosa0Jorge Simancas1Jose A. Vidal-Moya2Fernando Rey3Susana Valencia4Teresa Blasco5Instituto de Tecnología Química (UPV-CSIC), Universitat Politècnica de València, Consejo Superior de Investigaciones Científicas, Av. de los Naranjos s/n, 46022 Valencia, SpainInstituto de Tecnología Química (UPV-CSIC), Universitat Politècnica de València, Consejo Superior de Investigaciones Científicas, Av. de los Naranjos s/n, 46022 Valencia, SpainInstituto de Tecnología Química (UPV-CSIC), Universitat Politècnica de València, Consejo Superior de Investigaciones Científicas, Av. de los Naranjos s/n, 46022 Valencia, SpainInstituto de Tecnología Química (UPV-CSIC), Universitat Politècnica de València, Consejo Superior de Investigaciones Científicas, Av. de los Naranjos s/n, 46022 Valencia, SpainInstituto de Tecnología Química (UPV-CSIC), Universitat Politècnica de València, Consejo Superior de Investigaciones Científicas, Av. de los Naranjos s/n, 46022 Valencia, SpainInstituto de Tecnología Química (UPV-CSIC), Universitat Politècnica de València, Consejo Superior de Investigaciones Científicas, Av. de los Naranjos s/n, 46022 Valencia, SpainThe nature of organic structure directing agents (OSDAs) is of paramount importance in the final properties of zeolites, particularly the framework and porosity. Recently, the use of P-containing OSDAs has been employed for new zeolites, but there is little discussion compared to their analogues N-OSDAs. The main objective of this work is the characterization of pure silica MFI zeolite (silicalite-1) prepared by the <i>dual-template</i> route with tetrapropylammonium (TPA), tetrapropylphosphonium (TPP) cations, and mixtures thereof aiming to understand by advanced NMR methods how the nature of the organic influences the physico-chemical properties of the zeolite. Silicalite-1 has been successfully synthesized using the <i>dual-template</i> procedure with TPA and TPP molecules. Both OSDAs are incorporated into the zeolite without any specific preference, differently to that observed before for the TEA/TEP system, and homogenously mixed inside of the zeolite voids. The presence of TPP leads to the incorporation of less F, raising the concentration of Q<sup>3</sup>-defective sites in the silicalite-1 zeolites. Detailed NMR results indicate that those structural defects are close to the –CH<sub>3</sub> group of the entrapped OSDAs in the zeolite and these defects consist of at least two silanol groups stabilizing the Si-O<sup>-</sup> species, which is responsible for the charge balancing.https://www.mdpi.com/2076-3417/11/15/6850P-based OSDAszeolitessolid state MAS-NMR |
| spellingShingle | Joaquin Martinez-Ortigosa Jorge Simancas Jose A. Vidal-Moya Fernando Rey Susana Valencia Teresa Blasco A Multi-Nuclear MAS-NMR Study on the Structural Properties of Silicalite-1 Zeolite Synthesized Using N- and P-Based Organic Structure Directing Agents Applied Sciences P-based OSDAs zeolites solid state MAS-NMR |
| title | A Multi-Nuclear MAS-NMR Study on the Structural Properties of Silicalite-1 Zeolite Synthesized Using N- and P-Based Organic Structure Directing Agents |
| title_full | A Multi-Nuclear MAS-NMR Study on the Structural Properties of Silicalite-1 Zeolite Synthesized Using N- and P-Based Organic Structure Directing Agents |
| title_fullStr | A Multi-Nuclear MAS-NMR Study on the Structural Properties of Silicalite-1 Zeolite Synthesized Using N- and P-Based Organic Structure Directing Agents |
| title_full_unstemmed | A Multi-Nuclear MAS-NMR Study on the Structural Properties of Silicalite-1 Zeolite Synthesized Using N- and P-Based Organic Structure Directing Agents |
| title_short | A Multi-Nuclear MAS-NMR Study on the Structural Properties of Silicalite-1 Zeolite Synthesized Using N- and P-Based Organic Structure Directing Agents |
| title_sort | multi nuclear mas nmr study on the structural properties of silicalite 1 zeolite synthesized using n and p based organic structure directing agents |
| topic | P-based OSDAs zeolites solid state MAS-NMR |
| url | https://www.mdpi.com/2076-3417/11/15/6850 |
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