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

Author:

Pfriem Niklas1ORCID,Hintermeier Peter H.1,Eckstein Sebastian1ORCID,Kim Sungmin2ORCID,Liu Qiang13ORCID,Shi Hui14ORCID,Milakovic Lara1ORCID,Liu Yuanshuai15ORCID,Haller Gary L.1,Baráth Eszter1ORCID,Liu Yue1ORCID,Lercher Johannes A.12ORCID

Affiliation:

1. Department of Chemistry and Catalysis Research Center, Technical University of Munich, Lichtenbergstrasse 4, 85747 Garching, Germany.

2. Institute for Integrated Catalysis, Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352, USA.

3. Paul Scherrer Institute, Forschungsstrasse 111, 5232 Villigen PSI, Switzerland.

4. School of Chemistry and Chemical Engineering, Yangzhou University, Siwangting Road 180, 225009 Yangzhou, Jiangsu, China.

5. Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Songling Road 189, Laoshan District, Qingdao, China.

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

Funder

U.S. Department of Energy

Yale University

Publisher

American Association for the Advancement of Science (AAAS)

Subject

Multidisciplinary

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