NDLI: An examination of the intrinsic activity and stability of various solid acids during the catalytic decarboxylation of γ-valerolactone

Content Provider	Royal Society of Chemistry (RSC)
Author	Abdelrahman, Omar Ali Salary, Roozbeh Bond, Jesse Q. Kellicutt, Aimee B.
Copyright Year	2014
Abstract	Rates of γ-valerolactone (GVL) decarboxylation were measured in the gas phase under anhydrous conditions from 523–723 K over a series of solid acids including amorphous silica alumina, MFI zeolites, supported phosphotungstic acid, and γ-Al2O3. Through consideration of decarboxylation rates obtained under differential conditions, we examine the roles of Brønsted and Lewis acidity, deprotonation energy, and catalyst morphology in defining the intrinsic activity and stability of each material. In aluminosilicates, Brønsted sites associated with framework aluminum appear to contribute the majority of decarboxylation activity. Of the aluminosilicates tested, Brønsted sites in MFI are more intrinsically active than analogous sites in ASA; however, zeolite micropores hinder GVL diffusion and lead to mass transfer limitations at high temperatures. Relative to bridging hydroxyls, coordinatively unsaturated aluminum sites are substantially less active and do not contribute significantly to decarboxylation rates in materials having both framework and extraframework aluminum. Decarboxylation barriers scale with the deprotonation energy of Brønsted acid sites; however, lower deprotonation energies do not necessarily imply higher intrinsic activity in GVL decarboxylation. At 623 K, catalyst stability is highest in materials having large pore dimensions, Lewis sites as primary catalytic centers, and Brønsted sites with relatively high deprotonation energies.
Starting Page	2267
Ending Page	2279
Page Count	13
File Format	HTM / HTML PDF
ISSN	20444753
Volume Number	4
Issue Number	8
Journal	Catalysis Science & Technology
DOI	10.1039/c4cy00307a
Language	English
Publisher	Royal Society of Chemistry
Access Restriction	Open
Subject Keyword	Aluminium oxide MFI Gamma-Valerolactone Acid American National Standards Institute Lewis Decarboxylation Zeolite Diffusion Silicon dioxide Intrinsic activity Nsted
Content Type	Text
Resource Type	Article
Subject	Catalysis

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