Solvent-free conversion of CO2 in carbonates through a sustainable macroporous catalyst

被引:5
作者
Dattilo, Sandro [1 ]
Zagni, Chiara [2 ]
Mecca, Tommaso [3 ]
Patamia, Vincenzo [2 ]
Floresta, Giuseppe [2 ]
Nicotra, Pietro [4 ]
Carroccio, Sabrina C. [1 ]
Rescifina, Antonio [2 ]
机构
[1] Inst Polymers Composites & Biomat IPCB, CNR, Via Paolo Gaifami 18, I-95126 Catania, Italy
[2] Univ Catania, Dept Drug & Hlth Sci, Vle A Doria 6, I-95125 Catania, Italy
[3] Inst Biomol Chem ICB, CNR, Via Paolo Gaifami 18, I-95126 Catania, Italy
[4] Teamnetwork Srl, Via L Spagna 50-L-M, I-96100 Siracusa, Italy
关键词
Carbon dioxide; Heterogeneous catalysis; Cyclic carbonates; Metal-free catalysts; Hydrogen-bond donors; Tetramethylammonium cryrogel; CYCLIC CARBONATES; AMMONIUM-SALT; CHEMICAL FIXATION; EPOXIDES; DIOXIDE; SYSTEM; CYCLOADDITION; POLYMER; METRICS;
D O I
10.1016/j.giant.2024.100258
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
The novelty of this work consists of synthesizing and exploiting a heterogeneous catalyst containing ammonium chloride as part of the polymeric sponge sites for CO 2 capture. To this aim, the polymerization of 2-acryloyl(oxyethyl)trimethylammonium chloride was performed in cryo-condition, in the presence of a crosslinking agent, obtaining a lightweight macroporous freestanding material. Its efficiency in converting aromatic and aliphatic epoxides to the corresponding carbonates was successfully proved by using proton Nuclear Magnetic Resonance ( 1 H NMR). Remarkably, the conversion of styrene oxide (SO) to styrene carbonate (SC) reached a yield of 99 % after 24 h of reaction. The calculated yield versus the aliphatic cyclohexene oxide is 71 %. Similar results were obtained by substituting the resin counter anion with Br - , although the conversion kinetic was slower than the chloride. It is worth noticing that reactions took place in the mixture without adding the tetrabutylammonium bromide (TBAB), typically used as a co-catalyst to convert epoxides into carbonates. The recyclability of the as-prepared catalyst was evaluated for four reaction cycles, evidencing stable properties without significant depletion of CO 2 capture efficiency. Most importantly, the post-cleaning of the catalytic sponge is not required to be reused. Finally, the green chemistry metrics applied to the process demonstrated that our approach significantly mitigates risks and reduces environmental impact, thus elevating the overall cleanliness of our proof of concept.
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页数:11
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