通过可持续大孔催化剂实现碳酸盐中二氧化碳的无溶剂转化

IF 5.4 1区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY 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
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引用次数: 0

摘要

这项工作的新颖之处在于合成和利用了一种含有氯化铵的异相催化剂,作为用于捕获二氧化碳的聚合物海绵的一部分。为此,在交联剂的存在下,在低温条件下对 2-丙烯酰(氧乙基)三甲基氯化铵进行了聚合,从而获得了一种轻质大孔独立材料。质子核磁共振(1H NMR)成功证明了它将芳香族和脂肪族环氧化物转化为相应碳酸盐的效率。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%。脂肪族环己烯氧化物的计算收率为 71%。用 Br- 替代树脂反阴离子也得到了类似的结果,尽管转化动力学比氯化物慢。值得注意的是,反应是在混合物中进行的,没有添加通常用作将环氧化物转化为碳酸盐的辅助催化剂的四丁基溴化铵(TBAB)。对制备的催化剂进行了四个反应周期的可回收性评估,结果表明该催化剂性能稳定,二氧化碳捕获效率没有明显下降。最重要的是,催化海绵的后期清洁工作无需重复使用。最后,应用于该工艺的绿色化学指标表明,我们的方法大大降低了风险,减少了对环境的影响,从而提升了概念验证的整体清洁度。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

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

The novelty of this work consists of synthesizing and exploiting a heterogeneous catalyst containing ammonium chloride as part of the polymeric sponge sites for CO2 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 (1H 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 CO2 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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来源期刊
GIANT
GIANT Multiple-
CiteScore
8.50
自引率
8.60%
发文量
46
审稿时长
42 days
期刊介绍: Giant is an interdisciplinary title focusing on fundamental and applied macromolecular science spanning all chemistry, physics, biology, and materials aspects of the field in the broadest sense. Key areas covered include macromolecular chemistry, supramolecular assembly, multiscale and multifunctional materials, organic-inorganic hybrid materials, biophysics, biomimetics and surface science. Core topics range from developments in synthesis, characterisation and assembly towards creating uniformly sized precision macromolecules with tailored properties, to the design and assembly of nanostructured materials in multiple dimensions, and further to the study of smart or living designer materials with tuneable multiscale properties.
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