Prudent Choice of Iron‐Based Metal‐Organic Networks for Solvent‐Free CO2 Fixation at Ambient Pressure

• Published in: European journal of inorganic chemistry Vol. 2022; no. 13
• Main Authors: Mitra, Antarip, Biswas, Tanmoy, Ghosh, Sourav, Tudu, Gouri, Paliwal, Khushboo S., Ganatra, Pragati, Mahalingam, Venkataramanan
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 09-05-2022
• Subjects: Additives; Amorphous materials; Atmospheric pressure; Carbon dioxide; Carbon dioxide concentration; Carbon dioxide fixation; Carbon sequestration; Carbonates; Catalysts; Catalytic activity; Catechol; Climate change; Conversion; Cyclic carbonates; External pressure; Fixation; Heterogenous catalyst; Inorganic chemistry; Iron; Solvent-free; Solvents; Synergistic effect; Tactics
• ISSN: 1434-1948; 1099-0682
• DOI: 10.1002/ejic.202101039

The rising global warming and associated climate change demand efficient tactics to reduce CO2 concentration in the atmosphere. Conversion of epoxides to cyclic carbonates utilizing CO2 is a promising and sustainable approach towards CO2 fixation. However, the inert nature of CO2 and high activation energy requirement for the particular reaction necessitate the use of efficient catalysts. In this work, we have designed and developed a heterogeneous catalyst using catechol functionalized guanidinium based ligands (L1) and Fe(III) ions to perform the CO2 fixation reaction. The resulting amorphous material (Fe−L1) possesses metal‐organic network as revealed through different characterization methods. The optimized catalyst Fe−L1 is efficient for the conversion of a variety of epoxides into their corresponding cyclic carbonates in very good yield (>80 %). The reactions were performed under atmospheric pressure without solvent and external additives (e. g., TBAI or KI). The investigation of the mechanistic pathway indeed validates the synergistic effect of metal and halide ions that leads to the efficient conversion of different epoxides into cyclic carbonates. Furthermore, no significant loss in the catalytic activity of the Fe−L1 is noticed up to six cycles. The post catalytic analyses clearly indicate the robust nature of the catalyst. The developed one component bifunctional catalytic system can pave way towards transition to sustainable carbon capture and conversion.
The development of bifunctional catalyst (Fe−L1) by reaction of Fe(NO3)3 ⋅ 9H2O and Ligand (L1) to perform the CO2 fixation in epoxides. The as‐prepared catalyst (Fe−L1) carried out the reaction under atmospheric pressure in absence of solvent and external homogeneous additives. Overall, Fe−L1 is a heterogeneous catalyst which is highly selective and recyclable.