Brønsted acid sites based on penta-coordinated aluminum species
Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical industry. It is widely believed that BASs consist only of tetra-coordinated aluminum sites (Al IV ) with bridging OH groups in zeolites or ne...
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| Published in | Nature communications Vol. 7; no. 1; pp. 13820 - 5 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
London
Nature Publishing Group UK
15.12.2016
Nature Publishing Group Nature Portfolio |
| Subjects | |
| Online Access | Get full text |
| ISSN | 2041-1723 2041-1723 |
| DOI | 10.1038/ncomms13820 |
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| Abstract | Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical industry. It is widely believed that BASs consist only of tetra-coordinated aluminum sites (Al
IV
) with bridging OH groups in zeolites or nearby silanols on ASA surfaces. Here we report the direct observation in ASA of a new type of BAS based on penta-coordinated aluminum species (Al
V
) by
27
Al-{
1
H} dipolar-mediated correlation two-dimensional NMR experiments at high magnetic field under magic-angle spinning. Both BAS-Al
IV
and -Al
V
show a similar acidity to protonate probe molecular ammonia. The quantitative evaluation of
1
H and
27
Al sites demonstrates that BAS-Al
V
co-exists with BAS-Al
IV
rather than replaces it, which opens new avenues for strongly enhancing the acidity of these popular solid acids.
Until now, it has been believed that Brønsted acid sites in amorphous silica-alumina are formed from only tetra-coordinated (Al
IV
) sites. Here, the authors use
27
Al-{
1
H} correlation NMR experiments to identify a new Al
V
-based Brønsted acid site, with implications for increasing the acidity of solid acid catalysts. |
|---|---|
| AbstractList | Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical industry. It is widely believed that BASs consist only of tetra-coordinated aluminum sites (AlIV ) with bridging OH groups in zeolites or nearby silanols on ASA surfaces. Here we report the direct observation in ASA of a new type of BAS based on penta-coordinated aluminum species (AlV ) by 27 Al-{1 H} dipolar-mediated correlation two-dimensional NMR experiments at high magnetic field under magic-angle spinning. Both BAS-AlIV and -AlV show a similar acidity to protonate probe molecular ammonia. The quantitative evaluation of 1 H and 27 Al sites demonstrates that BAS-AlV co-exists with BAS-AlIV rather than replaces it, which opens new avenues for strongly enhancing the acidity of these popular solid acids. Until now, it has been believed that Brønsted acid sites in amorphous silica-alumina are formed from only tetra-coordinated (AlIV) sites. Here, the authors use 27Al-{1H} correlation NMR experiments to identify a new AlV-based Brønsted acid site, with implications for increasing the acidity of solid acid catalysts. Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical industry. It is widely believed that BASs consist only of tetra-coordinated aluminum sites (Al ) with bridging OH groups in zeolites or nearby silanols on ASA surfaces. Here we report the direct observation in ASA of a new type of BAS based on penta-coordinated aluminum species (Al ) by Al-{ H} dipolar-mediated correlation two-dimensional NMR experiments at high magnetic field under magic-angle spinning. Both BAS-Al and -Al show a similar acidity to protonate probe molecular ammonia. The quantitative evaluation of H and Al sites demonstrates that BAS-Al co-exists with BAS-Al rather than replaces it, which opens new avenues for strongly enhancing the acidity of these popular solid acids. Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical industry. It is widely believed that BASs consist only of tetra-coordinated aluminum sites (Al IV ) with bridging OH groups in zeolites or nearby silanols on ASA surfaces. Here we report the direct observation in ASA of a new type of BAS based on penta-coordinated aluminum species (Al V ) by 27 Al-{ 1 H} dipolar-mediated correlation two-dimensional NMR experiments at high magnetic field under magic-angle spinning. Both BAS-Al IV and -Al V show a similar acidity to protonate probe molecular ammonia. The quantitative evaluation of 1 H and 27 Al sites demonstrates that BAS-Al V co-exists with BAS-Al IV rather than replaces it, which opens new avenues for strongly enhancing the acidity of these popular solid acids. Until now, it has been believed that Brønsted acid sites in amorphous silica-alumina are formed from only tetra-coordinated (Al IV ) sites. Here, the authors use 27 Al-{ 1 H} correlation NMR experiments to identify a new Al V -based Brønsted acid site, with implications for increasing the acidity of solid acid catalysts. Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical industry. It is widely believed that BASs consist only of tetra-coordinated aluminum sites (AlIV) with bridging OH groups in zeolites or nearby silanols on ASA surfaces. Here we report the direct observation in ASA of a new type of BAS based on penta-coordinated aluminum species (AlV) by 27Al-{1H} dipolar-mediated correlation two-dimensional NMR experiments at high magnetic field under magic-angle spinning. Both BAS-AlIV and -AlV show a similar acidity to protonate probe molecular ammonia. The quantitative evaluation of 1H and 27Al sites demonstrates that BAS-AlV co-exists with BAS-AlIV rather than replaces it, which opens new avenues for strongly enhancing the acidity of these popular solid acids. Until now, it has been believed that Brønsted acid sites in amorphous silica-alumina are formed from only tetra-coordinated (AlIV) sites. Here, the authors use 27Al-{1H} correlation NMR experiments to identify a new AlV-based Brønsted acid site, with implications for increasing the acidity of solid acid catalysts. Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical industry. It is widely believed that BASs consist only of tetra-coordinated aluminum sites (AlIV) with bridging OH groups in zeolites or nearby silanols on ASA surfaces. Here we report the direct observation in ASA of a new type of BAS based on penta-coordinated aluminum species (AlV) by 27Al-{1H} dipolar-mediated correlation two-dimensional NMR experiments at high magnetic field under magic-angle spinning. Both BAS-AlIV and -AlV show a similar acidity to protonate probe molecular ammonia. The quantitative evaluation of 1H and 27Al sites demonstrates that BAS-AlV co-exists with BAS-AlIV rather than replaces it, which opens new avenues for strongly enhancing the acidity of these popular solid acids.Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical industry. It is widely believed that BASs consist only of tetra-coordinated aluminum sites (AlIV) with bridging OH groups in zeolites or nearby silanols on ASA surfaces. Here we report the direct observation in ASA of a new type of BAS based on penta-coordinated aluminum species (AlV) by 27Al-{1H} dipolar-mediated correlation two-dimensional NMR experiments at high magnetic field under magic-angle spinning. Both BAS-AlIV and -AlV show a similar acidity to protonate probe molecular ammonia. The quantitative evaluation of 1H and 27Al sites demonstrates that BAS-AlV co-exists with BAS-AlIV rather than replaces it, which opens new avenues for strongly enhancing the acidity of these popular solid acids. Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical industry. It is widely believed that BASs consist only of tetra-coordinated aluminum sites (Al IV ) with bridging OH groups in zeolites or nearby silanols on ASA surfaces. Here we report the direct observation in ASA of a new type of BAS based on penta-coordinated aluminum species (Al V ) by 27 Al-{ 1 H} dipolar-mediated correlation two-dimensional NMR experiments at high magnetic field under magic-angle spinning. Both BAS-Al IV and -Al V show a similar acidity to protonate probe molecular ammonia. The quantitative evaluation of 1 H and 27 Al sites demonstrates that BAS-Al V co-exists with BAS-Al IV rather than replaces it, which opens new avenues for strongly enhancing the acidity of these popular solid acids. |
| ArticleNumber | 13820 |
| Author | Jiang, Yijiao Lafon, Olivier Trébosc, Julien Wang, Zichun Stampfl, Catherine Baiker, Alfons Duk Kim, Kyung Amoureux, Jean-Paul Huang, Jun |
| Author_xml | – sequence: 1 givenname: Zichun surname: Wang fullname: Wang, Zichun organization: Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, Sydney University – sequence: 2 givenname: Yijiao surname: Jiang fullname: Jiang, Yijiao organization: Department of Engineering, Macquarie University – sequence: 3 givenname: Olivier surname: Lafon fullname: Lafon, Olivier organization: Univ. Lille, CNRS, UMR 8181-UCCS, Unité de Catalyse et de Chimie du Solide – sequence: 4 givenname: Julien surname: Trébosc fullname: Trébosc, Julien organization: Univ. Lille, CNRS, UMR 8181-UCCS, Unité de Catalyse et de Chimie du Solide – sequence: 5 givenname: Kyung surname: Duk Kim fullname: Duk Kim, Kyung organization: Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, Sydney University – sequence: 6 givenname: Catherine surname: Stampfl fullname: Stampfl, Catherine organization: School of Physics, Sydney University – sequence: 7 givenname: Alfons surname: Baiker fullname: Baiker, Alfons organization: Department of Chemistry and Applied Bioscience, Institute for Chemical and Bioengineering, ETH Zürich, Hönggerberg, HCI – sequence: 8 givenname: Jean-Paul surname: Amoureux fullname: Amoureux, Jean-Paul email: jun.huang@sydney.edu.au organization: Univ. Lille, CNRS, UMR 8181-UCCS, Unité de Catalyse et de Chimie du Solide – sequence: 9 givenname: Jun surname: Huang fullname: Huang, Jun email: jean-paul.amoureux@univ-lille1.fr organization: Laboratory for Catalysis Engineering, School of Chemical and Biomolecular Engineering, Sydney University |
| BackLink | https://www.ncbi.nlm.nih.gov/pubmed/27976673$$D View this record in MEDLINE/PubMed https://hal.science/hal-01796012$$DView record in HAL |
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| Snippet | Zeolites and amorphous silica-alumina (ASA), which both provide Brønsted acid sites (BASs), are the most extensively used solid acid catalysts in the chemical... Until now, it has been believed that Brønsted acid sites in amorphous silica-alumina are formed from only tetra-coordinated (AlIV) sites. Here, the authors use... |
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| SubjectTerms | 140/131 639/638/11/878 639/638/263 639/638/77 639/638/911 Acidity Aluminum Aluminum oxide Ammonia Catalysts Chemical industry Chemical Sciences Humanities and Social Sciences Magnetic fields Material chemistry multidisciplinary NMR Nuclear magnetic resonance Organic chemistry Quantitative analysis Science Science (multidisciplinary) Silica Silicon dioxide Zeolites |
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| Title | Brønsted acid sites based on penta-coordinated aluminum species |
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