Role of the ionic environment in enhancing the activity of reacting molecules in zeolite pores
Abstract
Speeding reactions through ionic strength: Brønsted acidity is introduced into microporous zeolites through the addition of framework aluminum. Pfriem et al. show that in the presence of water, the limited volume in the microchannels of zeolite H-MFI leads to a high concentration of hydrated hydronium ions at aluminum sites. The resulting high charge density creates a highly non-ideal solvation environment and, for cyclohexanol dehydrogenation, the charged carbenium-ion transition state was stabilized. A higher rate was maintained with lower-acidity sodium ion–exchanged zeolites that had the same high ionic strength. Science , abh3418, this issue p. 952
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The interaction between BAS zeolites and water governs proton solvation and thus acidity.
“This relationship governs many features of BAS zeolites including (i) proton solvation, and thus acidity7,8”
From A reactive neural network framework for water-loaded acidic zeolites (2024) · cites this paper as [7]
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Water-assisted shape-selective production of ethene in methanol-to-olefins reaction on SAPO-34
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Kinetics of Heterogeneous Single‐Site Catalysis
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Interactions of Polar and Nonpolar Groups of Alcohols in Zeolite Pores
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Impact of the Environment of BEA-Type Zeolites for Sorption of Water and Cyclohexanol
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Advances in the Synthesis of Crystalline Metallosilicate Zeolites via Interlayer Expansion
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- Authors
- Pfriem, N., Hintermeier, P. H., Eckstein, S., Kim, S., Liu, Q., Shi, H., Milakovic, L., Liu, Y., Haller, G. L., Baráth, E., Liu, Y., & Lercher, J. A.
- Affiliations
- Technical University of Munich (DE)
- Pacific Northwest National Laboratory (US)
- Paul Scherrer Institute (CH)
- Department of Chemistry and Catalysis Research Center, Technical University of Munich, Lichtenbergstrasse 4, 85747 Garching, Germany.
- Chinese Academy of Sciences (CN)
- Corresponding author
- Liu, Yue
- Lercher, Johannes A.
- ORCID
- Venue
- Science
- Published
- 2021-05-28
- Volume
- 372
- Issue
- 6545
- Pages
- 952-957
- ISSN
- 0036-8075 (ISSN-L)
- 1095-9203
- OpenAlex
- W3159861524
- Cited by
- 164
- References
- 29
- Citations by year
- 2026: 19 · 2025: 35 · 2024: 25 · 2023: 33 · 2022: 34 · 2021: 18
- FWCI
- 8.89
- Type
- journal article
- Language
- en
- Open access
- closed
- Locations
- Science (publishedVersion)
- PubMed (publishedVersion)
- DORA PSI (Paul Scherrer Institute) (submittedVersion)
- OSTI OAI (U.S. Department of Energy Office of Scientific and Technical Information) (submittedVersion)
- Funders
- U.S. Department of Energy (FWP 47319, DE-FG02-01ER15183)
- Yale University (CT 06520)
- Topics
- Physical Sciences › Chemistry › Inorganic Chemistry › Zeolite Catalysis and Synthesis
- Physical Sciences › Chemistry › Organic Chemistry › Chemical Synthesis and Reactions
- Physical Sciences › Chemistry › Inorganic Chemistry › Metal-Organic Frameworks: Synthesis and Applications
- Keywords
- zeolite catalysis, ionic environment, ionic strength, zeolitic water, framework aluminum, cation-anion pairs, carbocation stabilization, transition state stabilization, cyclohexanol dehydration, reaction rate enhancement, local chemical potential
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