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Three Series of Sulfo‐Functionalized Mixed‐Linker CAU‐10 Analogues: Sorption Properties, Proton Conductivity, and Catalytic Activity
Author(s) -
Reimer Nele,
Bueken Bart,
Leubner Sebastian,
Seidler Christopher,
Wark Michael,
De Vos Dirk,
Stock Norbert
Publication year - 2015
Publication title -
chemistry – a european journal
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.687
H-Index - 242
eISSN - 1521-3765
pISSN - 0947-6539
DOI - 10.1002/chem.201501502
Subject(s) - crystallinity , catalysis , sorption , thermal stability , conductivity , chemistry , ethylene , dehydration , proton , ethanol , phase (matter) , crystallography , organic chemistry , adsorption , biochemistry , physics , quantum mechanics
Abstract Ten mixed‐linker metal–organic frameworks [Al(OH)( m ‐BDC‐X) 1− y ( m ‐BDC‐SO 3 H) y ] (H 2 BDC=1,3‐benzenedicarboxylic acid; X=H, NO 2 , OH) exhibiting the CAU‐10‐type structure were synthesized. The compounds can be grouped into three series according to the combination of ligands employed. The three series of compounds were obtained by employing different ratios of m ‐H 2 BDC‐X and m ‐H 2 BDC‐SO 3 Li. The resulting compounds, which are denoted CAU‐10‐H/S x , ‐N/S x and ‐O/S x , show exceptionally high thermal stability for sulfonated materials of up to 350 °C. Detailed characterization with special focus on polarity and acidity was performed, and the impact of the additional SO 3 H groups is clearly demonstrated by changes in the sorption affinities/capacities towards several gases and water vapor. In addition, selected samples were evaluated for proton conductivity and as catalysts for the gas‐phase dehydration of ethanol to ethylene. While only very low proton conductivities were observed, a pronounced increase in catalytic activity was achieved. Although reactions were performed at temperatures of 250 and 300 °C for more than 40 h, no desulfonation and no loss of crystallinity were observed, and stable ethanol conversion resulted. This demonstrates the high stability of this material.