Identifying Crystallographically Different Si−OH−Al Brønsted Acid Sites in LTA Zeolites
A clear understanding of the acidic properties of bridging Si−OH−Al groups containing crystallographically different oxygen atoms in zeolites is a prerequisite for optimizing their performance as industrial solid catalysts and developing new acid‐catalyzed reactions, but presents many challenges. He...
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| Veröffentlicht in: | Angewandte Chemie International Edition 2022-06, Vol.61 (24), p.e202203603-n/a |
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| creator | Ahn, Sang Hyun Wang, Qiang Wang, Yongxiang Chu, Yueying Deng, Feng Hong, Suk Bong |
| description | A clear understanding of the acidic properties of bridging Si−OH−Al groups containing crystallographically different oxygen atoms in zeolites is a prerequisite for optimizing their performance as industrial solid catalysts and developing new acid‐catalyzed reactions, but presents many challenges. Here, we report the direct observation of yet unrecognized bridging Si−OH−Al groups in the LTA zeolite whose oxygen atoms are crystallographically different from those of already known Brønsted acid sites. We also report that the creation of a crystallographically particular type of bridging OH groups in zeolites and its concentration and acid strength can vary strongly with the content and spatial distribution of framework Al atoms, thus being synthetic in nature, which has been rationalized in terms of the secondary building unit concept.
The existence of crystallographically different Si−OH−Al Brønsted acid sites in LTA zeolites has been identified using IR and 2D MAS NMR spectroscopy and DFT calculations. This has been successfully rationalized in terms of the secondary building unit concept. |
| doi_str_mv | 10.1002/anie.202203603 |
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The existence of crystallographically different Si−OH−Al Brønsted acid sites in LTA zeolites has been identified using IR and 2D MAS NMR spectroscopy and DFT calculations. This has been successfully rationalized in terms of the secondary building unit concept.</description><subject>Acidity</subject><subject>Acids</subject><subject>Aluminum</subject><subject>Catalysts</subject><subject>Chemical reactions</subject><subject>Crystallographically Distinct Oxygen Atoms</subject><subject>Crystallography</subject><subject>IR Spectroscopy</subject><subject>NMR Spectroscopy</subject><subject>Oxygen</subject><subject>Oxygen atoms</subject><subject>Silicon</subject><subject>Spatial distribution</subject><subject>Zeolites</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2022</creationdate><recordtype>article</recordtype><recordid>eNqFkLtOwzAUhi0EoqWwMqJILCwpjh1fMoZSaKWKDpQFIUV24hRXaVLsRChvwMzTsPMmPAmuWorEwnIuOt_5dc4PwGkA-wGE6FKUWvURRAhiCvEe6AYEBT5mDO-7OsTYZ5wEHXBk7cLxnEN6CDqYYAQpQl3wNM5UWeu81eXcG5jW1qIoqrkRq2edurL1rnWeK-Mg715_vb1PRy7EhXdlPj9KW6vMi1OduVmtrKdLbzKLvUdVFev-GBzkorDqZJt74OFmOBuM_Mn0djyIJ36KobsQ85QIyCMYcKJonkvpgsgpjzDMQolpSCThkjDBCGeRZCyUKaRZimSWQcVxD1xsdFememmUrZOltqkqClGqqrEJoqH7nIaYOvT8D7qoGlO66xxFoyjCIWeO6m-o1FTWGpUnK6OXwrRJAJO178na92Tnu1s428o2cqmyHf5jtAOiDfCqC9X-I5fEd-Phr_g3YeCQlA</recordid><startdate>20220613</startdate><enddate>20220613</enddate><creator>Ahn, Sang Hyun</creator><creator>Wang, Qiang</creator><creator>Wang, Yongxiang</creator><creator>Chu, Yueying</creator><creator>Deng, Feng</creator><creator>Hong, Suk Bong</creator><general>Wiley Subscription Services, Inc</general><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope><orcidid>https://orcid.org/0000-0002-2855-1600</orcidid></search><sort><creationdate>20220613</creationdate><title>Identifying Crystallographically Different Si−OH−Al Brønsted Acid Sites in LTA Zeolites</title><author>Ahn, Sang Hyun ; Wang, Qiang ; Wang, Yongxiang ; Chu, Yueying ; Deng, Feng ; Hong, Suk Bong</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c3033-38c5a0890185e6ffbb6ffaf68930d4b3645b58b57a75879b774bc06dc2bdd0e83</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2022</creationdate><topic>Acidity</topic><topic>Acids</topic><topic>Aluminum</topic><topic>Catalysts</topic><topic>Chemical reactions</topic><topic>Crystallographically Distinct Oxygen Atoms</topic><topic>Crystallography</topic><topic>IR Spectroscopy</topic><topic>NMR Spectroscopy</topic><topic>Oxygen</topic><topic>Oxygen atoms</topic><topic>Silicon</topic><topic>Spatial distribution</topic><topic>Zeolites</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ahn, Sang Hyun</creatorcontrib><creatorcontrib>Wang, Qiang</creatorcontrib><creatorcontrib>Wang, Yongxiang</creatorcontrib><creatorcontrib>Chu, Yueying</creatorcontrib><creatorcontrib>Deng, Feng</creatorcontrib><creatorcontrib>Hong, Suk Bong</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Ahn, Sang Hyun</au><au>Wang, Qiang</au><au>Wang, Yongxiang</au><au>Chu, Yueying</au><au>Deng, Feng</au><au>Hong, Suk Bong</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Identifying Crystallographically Different Si−OH−Al Brønsted Acid Sites in LTA Zeolites</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2022-06-13</date><risdate>2022</risdate><volume>61</volume><issue>24</issue><spage>e202203603</spage><epage>n/a</epage><pages>e202203603-n/a</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>A clear understanding of the acidic properties of bridging Si−OH−Al groups containing crystallographically different oxygen atoms in zeolites is a prerequisite for optimizing their performance as industrial solid catalysts and developing new acid‐catalyzed reactions, but presents many challenges. Here, we report the direct observation of yet unrecognized bridging Si−OH−Al groups in the LTA zeolite whose oxygen atoms are crystallographically different from those of already known Brønsted acid sites. We also report that the creation of a crystallographically particular type of bridging OH groups in zeolites and its concentration and acid strength can vary strongly with the content and spatial distribution of framework Al atoms, thus being synthetic in nature, which has been rationalized in terms of the secondary building unit concept.
The existence of crystallographically different Si−OH−Al Brønsted acid sites in LTA zeolites has been identified using IR and 2D MAS NMR spectroscopy and DFT calculations. This has been successfully rationalized in terms of the secondary building unit concept.</abstract><cop>Germany</cop><pub>Wiley Subscription Services, Inc</pub><pmid>35320622</pmid><doi>10.1002/anie.202203603</doi><tpages>4</tpages><edition>International ed. in English</edition><orcidid>https://orcid.org/0000-0002-2855-1600</orcidid></addata></record> |
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| subjects | Acidity Acids Aluminum Catalysts Chemical reactions Crystallographically Distinct Oxygen Atoms Crystallography IR Spectroscopy NMR Spectroscopy Oxygen Oxygen atoms Silicon Spatial distribution Zeolites |
| title | Identifying Crystallographically Different Si−OH−Al Brønsted Acid Sites in LTA Zeolites |
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