当前位置: X-MOL 学术Giant › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Solvent-free conversion of CO2 in carbonates through a sustainable macroporous catalyst
Giant Pub Date : 2024-04-04 , DOI: 10.1016/j.giant.2024.100258
Sandro Dattilo , Chiara Zagni , Tommaso Mecca , Vincenzo Patamia , Giuseppe Floresta , Pietro Nicotra , Sabrina C. Carroccio , Antonio Rescifina

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 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 (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 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.

中文翻译:

通过可持续大孔催化剂无溶剂转化碳酸盐中的二氧化碳

这项工作的新颖之处在于合成和开发一种非均相催化剂,该催化剂含有氯化铵作为用于二氧化碳捕获的聚合物海绵位点的一部分。为此,在交联剂存在下,在低温条件下进行2-丙烯酰基(氧乙基)三甲基氯化铵的聚合,获得轻质大孔独立式材料。通过质子核磁共振(H NMR)成功证明了其将芳香族和脂肪族环氧化物转化为相应碳酸酯的效率。值得注意的是,反应 24 小时后,氧化苯乙烯 (SO) 转化为碳酸苯乙烯 (SC) 的产率达到 99%。相对于脂肪族环氧环己烷的计算产率为71%。通过用 Br 取代树脂抗衡阴离子获得了类似的结果,尽管转化动力学比氯化物慢。值得注意的是,反应在混合物中发生,没有添加四丁基溴化铵(TBAB),通常用作将环氧化物转化为碳酸酯的助催化剂。对所制备的催化剂的可回收性进行了四个反应循环的评估,证明了稳定的性能,并且没有显着降低 CO 捕获效率。最重要的是,催化海绵清洗后不需要重复使用。最后,应用于该过程的绿色化学指标表明,我们的方法显着降低了风险并减少了对环境的影响,从而提高了我们概念验证的整体清洁度。
更新日期:2024-04-04
down
wechat
bug