Halogenated melamine formaldehyde polymers: Efficient, robust and cost-effective bifunctional catalysts for continuous production of cyclic carbonates via. CO2-epoxide cycloadditionShow others and affiliations
2024 (English)In: Applied Catalysis A: General, ISSN 0926-860X, E-ISSN 1873-3875, Vol. 675, article id 119634Article in journal (Refereed) Published
Abstract [en]
Halogenated porous melamine polymers were demonstrated as an efficient catalyst for CO2-epoxide cycloaddition, selectively (>99%) producing C3-C12 cyclic carbonates in excellent yields (upto 99%) under solvent and co-catalyst free conditions. The halogenated polymers outperformed benchmark catalysts incorporating only basic (N-doped carbon, ZIF-8, N-rich melamine polymer) or nucleophilic (TBAB, KI) sites. The superior catalytic performance of these inexpensive polymers was attributed to their unique surface chemistry incorporating abundant, stable basic N sites (amine N and protonated N) and nucleophilic (Cl-, Br- or I-) that enabled simultaneous activation of both epoxide and CO2 molecule (supported by kinetic and DFT studies). Further, among halogenated polymers a Br- containing material (PMFBr) presented highest activity owing to its balanced CO2-philicity and strong nucleophilicity. Most importantly, PMFBr was robust, reusable and maintained stable performance for continuous production of C3-C4 cyclic carbonate (120 oC, 0.3-0.83 h-1 WHSVepoxide and 15 bar) in a fixed-bed reactor during 60-190 h TOS.
Place, publisher, year, edition, pages
Elsevier, 2024. Vol. 675, article id 119634
Keywords [en]
CO2 utilization, Cyclic carbonate, Bifunctional catalyst, Continuous cyclic carbonate synthesis, Porous melamine formaldehyde polymer, DFT
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:umu:diva-221358DOI: 10.1016/j.apcata.2024.119634Scopus ID: 2-s2.0-85186488606OAI: oai:DiVA.org:umu-221358DiVA, id: diva2:1839638
2024-02-212024-02-212024-03-13Bibliographically approved