More Efficient Chemical Recycling of Poly(ethylene terephthalate) by Intercepting Intermediates.

IF 7.5 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY ChemSusChem Pub Date : 2024-10-04 DOI:10.1002/cssc.202301698
Shelby Watson-Sanders, Mark D Dadmun
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Abstract

The research presented in this paper offers insight into the availability of intermediates in the depolymerization of Polyethylene Terephthalate (PET) to be used as feedstocks to create value added products. Monitoring the dispersity, molecular weight, end groups, and crystallinity of reaction intermediates during the heterogeneous depolymerization of PET offer insight into the mechanism by which the polymer chains evolve during the reaction. Our results show dispersity decreases and crystallinity increases, while the yield of insoluble PET remains high early in the reaction. Our interpretation of this data depicts a mechanism where chain scission targets amorphous tie-chains between crystalline phases. Targeting the tie-chains lowers the Mn of the polymer without changing the amount of recovered polymer flake. Chain scission of tie-chains and isolating highly crystalline PET lowers the dispersity ((Đ)) of the polymer chains, as the size of the crystalline lamellae guide the molecular weight of the depolymerized oligomers.  When sufficient end groups of PET chains are converted to alcohol groups, the PET flakes break apart into highly crystalline and less disperse polymer. Our results also demonstrate that the oligomeric depolymerization intermediates are readily repolymerized, offering new opportunities to more effectively and efficiently chemically recycle PET.

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通过拦截中间体提高聚对苯二甲酸乙二醇酯的化学回收效率。
本文介绍的研究深入探讨了聚对苯二甲酸乙二酯(PET)解聚过程中作为原料生产高附加值产品的中间体的可用性。在 PET 的异构解聚过程中监测反应中间产物的分散性、分子量、端基和结晶度,有助于深入了解聚合物链在反应过程中的演变机制。我们的研究结果表明,分散度降低,结晶度增加,而在反应早期,不溶性 PET 的产量仍然很高。我们对这些数据的解释描述了一种机制,即链的断裂以结晶相之间的无定形连接链为目标。以连接链为目标可降低聚合物的锰含量,而不会改变回收聚合物薄片的数量。由于结晶薄片的尺寸会影响解聚后低聚物的分子量,因此拉杆链的链裂和高结晶 PET 的分离会降低聚合物链的分散性((Đ))。 当 PET 链上足够多的末端基团转化为醇基时,PET 片就会分解成结晶度高、分散性较差的聚合物。我们的研究结果还表明,低聚物解聚中间体很容易再聚合,这为更有效、高效地化学回收 PET 提供了新的机遇。
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来源期刊
ChemSusChem
ChemSusChem 化学-化学综合
CiteScore
15.80
自引率
4.80%
发文量
555
审稿时长
1.8 months
期刊介绍: ChemSusChem Impact Factor (2016): 7.226 Scope: Interdisciplinary journal Focuses on research at the interface of chemistry and sustainability Features the best research on sustainability and energy Areas Covered: Chemistry Materials Science Chemical Engineering Biotechnology
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Ionomer and Membrane Designs for Low-Temperature CO2 and CO Electrolysis. Deciphering electrocatalytic hydrogen production in water through a bioinspired water-stable copper(II) complex adorned with (N2S2)-donor sites. Mechanistic Study of the Electrochemical Reduction of CO2 in Aprotic Ionic Liquid in Air. More Efficient Chemical Recycling of Poly(ethylene terephthalate) by Intercepting Intermediates. Active Sites for CO2 Hydrogenation to Methanol: Mechanistic Insights and Reaction Control.
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