聚对苯二甲酸乙二醇酯塑料与琥珀酸酯-15共热解制备单芳烃

IF 6.2 2区化学 Q1 CHEMISTRY, ANALYTICAL

Journal of Analytical and Applied Pyrolysis Pub Date : 2025-08-05 DOI:10.1016/j.jaap.2025.107319

Huiyu Liu , Chengyu Li , Rui Shan , Jun Zhang , Haoran Yuan , Yong Chen

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引用次数: 0

摘要

系统研究了聚对苯二甲酸乙二醇酯（PET）与Amberlyst-15 （A15）共热解对提高单芳烃（MAHs）产量的影响。通过Py-GC/MS和TG-MS分析，确定A15中的磺酸基（-SO3H）是PET与A15协同作用的关键活性位点。Brønsted酸位的掺入将PET的解聚温度从430°C降低到350°C，并证明对PET单体的脱羧/加氢脱氧有效。PET和A15（1:1）在850℃下快速共热解（104℃/s） 20 s， MAHs产率为14.9 wt%，选择性为55.2% %。动力学分析进一步表明，与理论预测值（156.0 kJ/mol）相比，Eα平均活化能（65.8 kJ/mol）降低了42.2 %(65.8 kJ/mol)，反应早期和中期的能垒最低。值得注意的是，PET固有的氢缺乏限制了分子间的氢转移，使环境氢可用性成为调节酸介导的单体转化途径的关键。这项工作展示了将废弃PET和A15转化为高价值芳烃的可持续策略，同时阐明了酸介导的塑料升级回收共热解的机制见解。

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Co-pyrolysis of polyethylene terephthalate plastic and Amberlyst-15 towards monoaromatic hydrocarbons production

The co-pyrolysis of polyethylene terephthalate (PET) and Amberlyst-15 (A15) was systematically investigated to enhance monoaromatic hydrocarbons (MAHs) production. Sulfonic acid groups (–SO₃H) in A15 were identified as the critical active sites for the synergistic interactions between PET and A15, as confirmed by Py-GC/MS and TG-MS analysis. The incorporation of Brønsted acid sites lowered the depolymerization temperature of PET from 430 °C to 350 °C and demonstrated effective for the decarboxylation/hydrodeoxygenation of PET monomers. Fast co-pyrolysis (10⁴°C/s) of PET and A15 (1:1) at 850 °C for 20 s resulted in a MAHs yield of 14.9 wt% and a selectivity of 55.2 %. Kinetic analysis further revealed that the average activation energy (Eα) decreased by 42.2 % (65.8 kJ/mol) compared to theoretical predictions (156.0 kJ/mol), with the lowest energy barriers observed during the early- and medium-stage reaction progress. Notably, the inherent hydrogen deficiency of PET constrained the intermolecular hydrogen transfer, making environmental hydrogen availability a key for regulating acid-mediated monomer conversion pathways. This work demonstrates a sustainable strategy for valorizing waste PET and A15 into high-value aromatics while elucidating mechanistic insights into acid-mediated co-pyrolysis for plastic upcycling.

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来源期刊

Journal of Analytical and Applied Pyrolysis 化学-分析化学

CiteScore

9.10

自引率

11.70%

发文量

340

审稿时长

44 days

期刊介绍： The Journal of Analytical and Applied Pyrolysis (JAAP) is devoted to the publication of papers dealing with innovative applications of pyrolysis processes, the characterization of products related to pyrolysis reactions, and investigations of reaction mechanism. To be considered by JAAP, a manuscript should present significant progress in these topics. The novelty must be satisfactorily argued in the cover letter. A manuscript with a cover letter to the editor not addressing the novelty is likely to be rejected without review.