Cited by 164Zeolite Catalysis and SynthesisChemical Synthesis and ReactionsMetal-Organic Frameworks: Synthesis and Applications

Role of the ionic environment in enhancing the activity of reacting molecules in zeolite pores

Pfriem, Niklas, Hintermeier, Peter H., Eckstein, Sebastian, Kim, Sungmin, Liu, Qiang, Shi, Hui, Milakovic, Lara, Liu, Yuanshuai +4 more·2021·Science

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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Crossref · 10.1126/science.abh3418

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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”

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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.
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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