Incorporation of Mg/Al metal oxide into ionic liquids for CO2 capture and conversion into cyclic carbonate under solvent-free conditions: effect of coordination ability, recyclability, and catalytic study

The direct conversion of carbon dioxide (CO 2 ) and propylene oxide (PO) into propylene carbonate (PC) offers a green way to utilize anthropogenic CO 2 . However, this reaction is limited by low conversion of PO and harsh reaction conditions. In this study, we solve this problem using ionic liquids (ILs)/metal oxide composites (ILs@MAO). The catalytic activity of MAO-500 (500 = annealing temperature) is poor evidenced by its low conversion of PO (24.94%). However, ILs@MAO-500 has a high conversion of PO (97.54%) under similar reaction conditions (2 h at 1.5 MPa CO 2 pressure, 90 o C, and 0.85 g catalyst). The ILs consist of imidazolium cation with weak coordinated [NTf 2 ] - anion leading to outward movement of anion resulting in the formation of “heterodinuclear complex”. This complex generates an amorphous-crystalline intermediate with balanced acid-base sites that activate PO and stabilize the catalytic intermediate. The high PO conversion is theorized to be primarily due to in large part the abundant reactive sites in the ILs that are covalently immobilized on the MAO-500 carrier. Furthermore, even after multiple recycling, ILs@MAO-500 remains stable and exhibits high yield and selectivity. The proposed solvent-free catalytic system is mild, kinetically fast, and naturally safe for coupling CO 2 and PO into PC synthesis. • Carbon dioxide (CO 2 ) is converted into a green chemical compound. • Good leaving group of an ionic liquid aids in the conversion of reactant. • A “heteronuclear complex” is formed between an ionic liquid and metal oxide. • Suppression of byproducts and increment of TON at optimum reaction condition. • Remarkable conversion retention of 88.4% after six recycle reactions.

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Publication Details

Journal
Green Chemical Engineering
Published
2024-10-09
DOI
https://doi.org/10.1016/j.gce.2024.10.002
Citations
3
Primary Topic
Carbon dioxide utilization in catalysis
Type
article
Field-Weighted Citation Impact
0.53

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article

Incorporation of Mg/Al metal oxide into ionic liquids for CO2 capture and conversion into cyclic carbonate under solvent-free conditions: effect of coordination ability, recyclability, and catalytic study

Hern Kim, Atul A. Pawar, Shimelis Kebede Kassahun, S. Anuradha Jabasingh
3 citations
Green Chemical Engineering
Carbon dioxide utilization in catalysis
0.53
article

Incorporation of Mg/Al metal oxide into ionic liquids for CO2 capture and conversion into cyclic carbonate under solvent-free conditions: effect of coordination ability, recyclability, and catalytic study

Hern Kim, Atul A. Pawar, Shimelis Kebede Kassahun, S. Anuradha Jabasingh
article en
3 citations

Abstract

The direct conversion of carbon dioxide (CO 2 ) and propylene oxide (PO) into propylene carbonate (PC) offers a green way to utilize anthropogenic CO 2 . However, this reaction is limited by low conversion of PO and harsh reaction conditions. In this study, we solve this problem using ionic liquids (ILs)/metal oxide composites (ILs@MAO). The catalytic activity of MAO-500 (500 = annealing temperature) is poor evidenced by its low conversion of PO (24.94%). However, ILs@MAO-500 has a high conversion of PO (97.54%) under similar reaction conditions (2 h at 1.5 MPa CO 2 pressure, 90 o C, and 0.85 g catalyst). The ILs consist of imidazolium cation with weak coordinated [NTf 2 ] - anion leading to outward movement of anion resulting in the formation of “heterodinuclear complex”. This complex generates an amorphous-crystalline intermediate with balanced acid-base sites that activate PO and stabilize the catalytic intermediate. The high PO conversion is theorized to be primarily due to in large part the abundant reactive sites in the ILs that are covalently immobilized on the MAO-500 carrier. Furthermore, even after multiple recycling, ILs@MAO-500 remains stable and exhibits high yield and selectivity. The proposed solvent-free catalytic system is mild, kinetically fast, and naturally safe for coupling CO 2 and PO into PC synthesis. • Carbon dioxide (CO 2 ) is converted into a green chemical compound. • Good leaving group of an ionic liquid aids in the conversion of reactant. • A “heteronuclear complex” is formed between an ionic liquid and metal oxide. • Suppression of byproducts and increment of TON at optimum reaction condition. • Remarkable conversion retention of 88.4% after six recycle reactions.

Green Chemical EngineeringVol. 7(1)
Addis Ababa Science and Technology University (ET), Addis Ababa University (ET), Myongji University (KR)
Ministry of Education, National Research Foundation of Korea
Openalex Percentile: Top 45%
Carbon dioxide utilization in catalysis
0.53
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