Tunning catalytic centers in heterogeneous catalyst, both in a chemical and a spatial manner, is a powerful approach to improve the stability and the efficiency of catalysts. While the chemical… Click to show full abstract
Tunning catalytic centers in heterogeneous catalyst, both in a chemical and a spatial manner, is a powerful approach to improve the stability and the efficiency of catalysts. While the chemical aspects are largely understood, the spatial interactions around active sites, comprised of non-covalent interactions, are difficult to maintain and challenging to study. Herein, we utilize the unique properties of covalent organic frameworks (COFs) to establish an ideal reaction environment for the hydrolysis of cellobiose and other common disaccharides in mild, metal-free, neutral aqueous conditions. The chosen COF, HCl-PSA-IM-COF-OMe, is modified to be ultra-stable in aqueous conditions and possesses sulfonic acid groups for general acid catalysis and for enhanced hydrogen bonding with reactants as well as intraporous chloride anions for oxocarbenium intermediate stabilization. In addition, the system also relies on the differences in adsorptive binding behavior, Kads , of the reactants and the products to the functionalized framework and benefits from a separate physical, kinetic process to boost the catalytic cycle. Due to its stability in aqueous conditions, HCl-PSA-IM-COF-OMe can be recycled and maintain its hydrolytic properties for five cycles before regeneration is needed. This article is protected by copyright. All rights reserved.
               
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