Metal organic polymer assisted halide free CO2 fixation into epoxides

Pan, Pratyay (2025) Metal organic polymer assisted halide free CO2 fixation into epoxides. Masters thesis, Indian Institute of Science Education and Research Kolkata.

Text (MS Dissertation of Pratyay Pan (23MP013)) 23MP013_Thesis_file.pdf - Submitted Version Restricted to Repository staff only Download (2MB)

Abstract

In context of carbon capture and utilization (CCU), utilizing CO2 as a C1 feedstock and converting it into value-added product (referred as CO2 fixation) is a widespread approach, to address excessive CO2 emission. Fixing CO2 into epoxides leads to generation of cyclic carbonates which holds promising application towards various Industrial sectors. Majority of the existing literatures reported the use of transition-metal base materials, in conjunction with detrimental halide-containing co-catalysts to catalysed this reaction. In this scenario, to overcome the limitation i.e. to get rid of the toxic halides, we synthesized a metal-organic polymer (Fe-PDC), using cheap and earth abundant materials through simple one step solvothermal process. The synthesized material shows efficiency towards halide-free CO2 fixation into epoxides to generate cyclic carbonates under mild and solvent-free conditions. Sophisticated spectroscopic techniques unravel that iron in +2 oxidation state binds with carboxylic group of PDC (2,5-pyridinedicarboxyliz acid). In the mechanistic investigation the Lewis acidic interaction between the catalyst and epoxide has been experimentally proved using 1H-NMR technique. Additionally, pyridine nitrogen might activate CO2 via carbamate anion formation and thus these overall processes smoothly accelerate the reaction. In presence of Fe-PDC, reaction shows 90% conversion with epichlorohydrin (ECH) in optimized reaction conditions. Consequently, this study highlights a promising approach of designing halide free catalytic system in promoting sustainable catalysis for synthesizing cyclic carbonates using CO2 and epoxide.

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