Degradation of polycarbonate waste to recover bisphenol A and dimethyl carbonate using urea as a cheap green catalyst†

IF 9.3 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Green Chemistry Pub Date : 2024-08-27 DOI:10.1039/d4gc03205e
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Abstract

Various excellent catalysts have been explored for the methanolysis of polycarbonate (PC), but it is still challenging to develop green and economical catalysts for solvent-free PC methanolysis to recover both bisphenol A (BPA) and dimethyl carbonate (DMC). Herein, green, efficient and solvent-free degradation of PC to BPA and DMC was achieved using urea as a cheap green catalyst. At 140 °C for 3 h, PC was completely degraded to BPA and DMC with yields of 93.4% and 74.7%, respectively. A possible catalytic degradation mechanism of PC was proposed by kinetic experiments and NMR, where urea, methanol and carbonate formed a six-membered ring in the reaction. It was found that the increase of urea concentration significantly reduced the activation energy, which was attributed to the fact that the increase of urea concentration made the six-membered ring easier to form and activated the carbonate bond. The degradation system can be reused directly up to 10 times and 100% degradation rate can be maintained. This work provides a simple, green and economical method for industrial PC recycling.

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使用尿素作为廉价绿色催化剂降解聚碳酸酯废料以回收双酚 A 和碳酸二甲酯
人们已探索出多种用于聚碳酸酯(PC)甲醇分解的优良催化剂,但开发绿色、经济的无溶剂 PC 甲醇分解催化剂以同时回收双酚 A(BPA)和碳酸二甲酯(DMC)仍是一项挑战。在此,使用尿素作为廉价的绿色催化剂,实现了 PC 向双酚 A 和 DMC 的绿色、高效和无溶剂降解。在 140 °C、3 小时的条件下,PC 被完全降解为双酚 A 和二甲基甲酰胺,产率分别为 93.4% 和 74.7%。通过动力学实验和核磁共振,提出了一种可能的 PC 催化降解机理,即尿素、甲醇和碳酸盐在反应中形成一个六元环。实验发现,尿素浓度的增加会显著降低活化能,这是因为尿素浓度的增加使六元环更容易形成,并激活了碳酸键。该降解系统可直接重复使用达 10 次,并能保持 100% 的降解率。这项工作为工业 PC 回收提供了一种简单、绿色和经济的方法。
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来源期刊
Green Chemistry
Green Chemistry 化学-化学综合
CiteScore
16.10
自引率
7.10%
发文量
677
审稿时长
1.4 months
期刊介绍: Green Chemistry is a journal that provides a unique forum for the publication of innovative research on the development of alternative green and sustainable technologies. The scope of Green Chemistry is based on the definition proposed by Anastas and Warner (Green Chemistry: Theory and Practice, P T Anastas and J C Warner, Oxford University Press, Oxford, 1998), which defines green chemistry as the utilisation of a set of principles that reduces or eliminates the use or generation of hazardous substances in the design, manufacture and application of chemical products. Green Chemistry aims to reduce the environmental impact of the chemical enterprise by developing a technology base that is inherently non-toxic to living things and the environment. The journal welcomes submissions on all aspects of research relating to this endeavor and publishes original and significant cutting-edge research that is likely to be of wide general appeal. For a work to be published, it must present a significant advance in green chemistry, including a comparison with existing methods and a demonstration of advantages over those methods.
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