MOF-based heterogeneous catalysis in continuous flow via incorporation onto polymer-based spherical activated carbon supports

• Published in: Nanoscale 2023-11, Vol.15 (44), p.17910-17921
• Main Authors: Griffiths, Anthony, Boyall, Sarah L., Müller, Pia, Harrington, John P., Sobolewska, Anna M., Reynolds, William R., Bourne, Richard A., Wu, Kejun, Collins, Sean M., Muldowney, Mark, Chamberlain, Thomas W.
• Format: Article
• Language: English
• Subjects: Absorption spectroscopy; Activated carbon; Catalysis; Catalysts; Catalytic activity; Chemical reactions; Citronellal; Composite materials; Continuous flow; Crush tests; Energy dispersive X ray analysis; Ion beams; Lewis acid; Metal-organic frameworks; Nanomaterials; Polymers; Thermogravimetric analysis; X ray analysis; X ray powder diffraction
• ISSN: 2040-3364; 2040-3372
• DOI: 10.1039/d3nr03634k

We present an approach to harnessing the tuneable catalytic properties of complex nanomaterials for continuous flow heterogeneous catalysis by combining them with the scalable and industrially implementable properties of carbon pelleted supports. This approach, in turn, will enable these catalytic materials, which largely currently exist in forms unsuitable for this application ( e.g. powders), to be fully integrated into large scale, chemical processes. A composite heterogeneous catalyst consisting of a metal–organic framework-based Lewis acid, MIL-100(Sc), immobilised onto polymer-based spherical activated carbon (PBSAC) support has been developed. The material was characterised by focused ion beam-scanning electron microscopy-energy dispersive X-ray analysis, powder X-ray diffraction, N 2 adsorption, thermogravimetric analysis, atomic absorption spectroscopy, light scattering and crush testing with the catalytic activity studied in continuous flow. The mechanically robust spherical geometry makes the composite material ideal for application in packed-bed reactors. The catalyst was observed to operate without any loss in activity at steady state for 9 hours when utilised as a Lewis acid catalyst for the intramolecular cyclisation of (±)-citronellal as a model reaction. This work paves the way for further development into the exploitation of MOF-based continuous flow heterogeneous catalysis.