Stability of Zeolites in Aqueous Phase Reactions.
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| Title: | Stability of Zeolites in Aqueous Phase Reactions. |
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| Authors: | Prodinger, Sebastian1, Hui Shi1, Eckstein, Sebastian2, Jian Zhi Hu1, Olarte, Mariefel V.1, Camaioni, Donald M.1, Derewinski, Miroslaw A.1 miroslaw.derewinski@pnnl.gov, Lercher, Johannes A.1,2 Johannes.Lercher@pnnl.gov |
| Source: | Chemistry of Materials. Sep2017, Vol. 29, p7255-7262. 8p. |
| Subjects: | Molecular structure of zeolites, Chemical modification of proteins, Oxonium ions, Cyclohexanols, Zeolite catalysts |
| Abstract: | Strategies to understand and mitigate the corrosive interactions of zeolites in aqueous phase under reaction conditions have been explored using zeolite BEA as an example. The states of Si and Al atoms after chemical modification and during gradual degradation were followed by cross-polarization enhanced 29Si MAS NMR and 27Al MAS NMR as well as IR spectroscopy. The key to stabilizing a zeolite for aqueous phase catalysis is to reduce the pore concentration of water in the presence of reacting substrates. The concentration of tetrahedral aluminum, which is charge balanced by hydrated hydronium ions, is the most important parameter determining the concentration of water in the zeolite pores. Lower intraporous water concentrations, largely independent of ubiquitous defects, led to longer zeolite lifetimes during cyclohexanol dehydration. The concentration of intraporous water was directly related to the rate of hydrolysis of Si4+ from the zeolite lattice and its removal from the crystal. Dissolution of Si4+ led eventually to a loss of confinement of the catalytically active hydronium ions and decreased the catalytic activity. At low Brønsted acid site concentrations, water bound to lattice defects begins to exert a measurable influence on the stability under reaction conditions. [ABSTRACT FROM AUTHOR] |
| Copyright of Chemistry of Materials is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.) | |
| Database: | Engineering Source |
| FullText | Text: Availability: 0 |
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| Header | DbId: egs DbLabel: Engineering Source An: 126070251 AccessLevel: 6 PubType: Academic Journal PubTypeId: academicJournal PreciseRelevancyScore: 0 |
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| Items | – Name: Title Label: Title Group: Ti Data: Stability of Zeolites in Aqueous Phase Reactions. – Name: Author Label: Authors Group: Au Data: <searchLink fieldCode="AR" term="%22Prodinger%2C+Sebastian%22">Prodinger, Sebastian</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Hui+Shi%22">Hui Shi</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Eckstein%2C+Sebastian%22">Eckstein, Sebastian</searchLink><relatesTo>2</relatesTo><br /><searchLink fieldCode="AR" term="%22Jian+Zhi+Hu%22">Jian Zhi Hu</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Olarte%2C+Mariefel+V%2E%22">Olarte, Mariefel V.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Camaioni%2C+Donald+M%2E%22">Camaioni, Donald M.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Derewinski%2C+Miroslaw+A%2E%22">Derewinski, Miroslaw A.</searchLink><relatesTo>1</relatesTo><i> miroslaw.derewinski@pnnl.gov</i><br /><searchLink fieldCode="AR" term="%22Lercher%2C+Johannes+A%2E%22">Lercher, Johannes A.</searchLink><relatesTo>1,2</relatesTo><i> Johannes.Lercher@pnnl.gov</i> – Name: TitleSource Label: Source Group: Src Data: <searchLink fieldCode="JN" term="%22Chemistry+of+Materials%22">Chemistry of Materials</searchLink>. Sep2017, Vol. 29, p7255-7262. 8p. – Name: Subject Label: Subjects Group: Su Data: <searchLink fieldCode="DE" term="%22Molecular+structure+of+zeolites%22">Molecular structure of zeolites</searchLink><br /><searchLink fieldCode="DE" term="%22Chemical+modification+of+proteins%22">Chemical modification of proteins</searchLink><br /><searchLink fieldCode="DE" term="%22Oxonium+ions%22">Oxonium ions</searchLink><br /><searchLink fieldCode="DE" term="%22Cyclohexanols%22">Cyclohexanols</searchLink><br /><searchLink fieldCode="DE" term="%22Zeolite+catalysts%22">Zeolite catalysts</searchLink> – Name: Abstract Label: Abstract Group: Ab Data: Strategies to understand and mitigate the corrosive interactions of zeolites in aqueous phase under reaction conditions have been explored using zeolite BEA as an example. The states of Si and Al atoms after chemical modification and during gradual degradation were followed by cross-polarization enhanced 29Si MAS NMR and 27Al MAS NMR as well as IR spectroscopy. The key to stabilizing a zeolite for aqueous phase catalysis is to reduce the pore concentration of water in the presence of reacting substrates. The concentration of tetrahedral aluminum, which is charge balanced by hydrated hydronium ions, is the most important parameter determining the concentration of water in the zeolite pores. Lower intraporous water concentrations, largely independent of ubiquitous defects, led to longer zeolite lifetimes during cyclohexanol dehydration. The concentration of intraporous water was directly related to the rate of hydrolysis of Si4+ from the zeolite lattice and its removal from the crystal. Dissolution of Si4+ led eventually to a loss of confinement of the catalytically active hydronium ions and decreased the catalytic activity. At low Brønsted acid site concentrations, water bound to lattice defects begins to exert a measurable influence on the stability under reaction conditions. [ABSTRACT FROM AUTHOR] – Name: AbstractSuppliedCopyright Label: Group: Ab Data: <i>Copyright of Chemistry of Materials is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.) |
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| RecordInfo | BibRecord: BibEntity: Identifiers: – Type: doi Value: 10.1021/acs.chemmater.7b01847 Languages: – Code: eng Text: English PhysicalDescription: Pagination: PageCount: 8 StartPage: 7255 Subjects: – SubjectFull: Molecular structure of zeolites Type: general – SubjectFull: Chemical modification of proteins Type: general – SubjectFull: Oxonium ions Type: general – SubjectFull: Cyclohexanols Type: general – SubjectFull: Zeolite catalysts Type: general Titles: – TitleFull: Stability of Zeolites in Aqueous Phase Reactions. Type: main BibRelationships: HasContributorRelationships: – PersonEntity: Name: NameFull: Prodinger, Sebastian – PersonEntity: Name: NameFull: Hui Shi – PersonEntity: Name: NameFull: Eckstein, Sebastian – PersonEntity: Name: NameFull: Jian Zhi Hu – PersonEntity: Name: NameFull: Olarte, Mariefel V. – PersonEntity: Name: NameFull: Camaioni, Donald M. – PersonEntity: Name: NameFull: Derewinski, Miroslaw A. – PersonEntity: Name: NameFull: Lercher, Johannes A. IsPartOfRelationships: – BibEntity: Dates: – D: 12 M: 09 Text: Sep2017 Type: published Y: 2017 Identifiers: – Type: issn-print Value: 08974756 Numbering: – Type: volume Value: 29 Titles: – TitleFull: Chemistry of Materials Type: main |
| ResultId | 1 |
