Shaping MOF oxime oxidation catalysts as three-dimensional porous aerogels through structure-directing growth inside chitosan microspheres

Autor: Nisrine Hammi, Shuo Chen, Ana Primo, Sebastien Royer, Hermenegildo Garcia, Abdelkrim El Kadib
Rok vydání: 2022
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Zdroj: Digital.CSIC. Repositorio Institucional del CSIC
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ISSN: 1463-9270
Popis: Metal-organic frameworks stand as unique building blocks, bridging the gap between coordination chemistry and materials science. While significant advances have been made in their design, current efforts focus on expanding their pore size above the microporous regime and on their shaping into well suitable end use devices. For such a purpose, we herein explored the use of chitosan hydrogel microspheres as a mold to grow an extended network of MOFs, followed by CO-supercritical drying to generate three-dimensional polysaccharide nanofibrils embedding entangled MOF nanoclusters. This strategy was found to be highly versatile, and allows for shaping HKUST-1, ZIF-8, ZIF-67 and Fe-BTC inside chitosan microspheres. The resulting lightweight aerogels display excellent activity for oxime oxidation, with HKUST-1 loaded on chitosan beads standing as the most promising. The virtues of supercritical drying were substantiated by comparing the catalytic activity of these aerogels with their xerogel analogues as well as pristine HKUST-1. Interestingly, moreover, the configuration of MOFs in chitosan beads precludes the metal from leaching and allows easy recovery of the catalyst from the medium and its possible recycling.
NH thanks UEMF and UPV for an Erasmus+ 2019-1-ES01-KA107-062073 Scholarship. AEK thanks UEMF for funding. Partenariat Hubert Curien – Toubkal (project no. 18/70) is acknowledged for supporting and partially funding this work. Chevreul Institute (FR 2638), Ministère de l'Enseignement Supérieur et de la Recherche, Région Hauts-de-France and FEDER are acknowledged for funding. The authors are also thankful for the technical support from Lille University: Martine Trentesaux and Pardis Simon for the XPS analysis, Olivier Gardoll for the TGA analysis, Laurence Burylo for the XRD experiments, and Jeremy Dhainaut for the mechanical tests, and Ridvan Yildiz from LMCPA, Hauts de France Polytechnic University for mercury intrusion.
Databáze: OpenAIRE