温和条件下氯化镓基熔融盐催化聚烯烃与聚苯乙烯无溶剂化学回收

doi:10.1016/S1872-2067(26)65067-X

催化学报 ›› 2026, Vol. 86: 137-148.DOI: 10.1016/S1872-2067(26)65067-X

温和条件下氯化镓基熔融盐催化聚烯烃与聚苯乙烯无溶剂化学回收

袁磊^a, 高志文^a, 石利斌^b, 管翠诗^b, 彭东岳^b^,^*(), 方淑慧^a, 章伟^a^,^c^,^d^,^*(), 刘玥^a^,^c^,^*()

^a 华东师范大学化学与分子工程学院, 石油化工分子转化与反应工程全国重点实验室, 上海市绿色化学与化工过程绿色化重点实验室, 上海 200062
^b 中石化石油化工科学研究院有限公司, 石油化工分子转化与反应工程全国重点实验室, 北京 100083
^c 华东师范大学, 可再生碳资源科学与技术工程中心, 上海 200241
^d 上海理工大学光化学与光材料研究院, 材料与化学学院, 上海 200093

收稿日期:2025-11-03 接受日期:2026-01-06 出版日期:2026-07-05 发布日期:2026-06-12
通讯作者: ^*电子信箱: pengdongyue.ripp@sinopec.com (彭东岳),
weizhang@chem.ecnu.edu.cn (章伟),
liuyue@chem.ecnu.edu.cn (刘玥).
基金资助:
中石化石油化工科学研究院有限公司资助科研项目(36800000-24-ZC0613-0023);国家自然科学基金(22472059);国家自然科学基金(22302069);国家自然科学基金(22309212);上海市自然科学基金(23ZR1418800);上海市科技创新生态建设计划(25520750100)

Solvent-free chemical recycling of polyolefins and polystyrene under mild conditions via GaCl₃-based molten catalysts

Lei Yuan^a, Zhiwen Gao^a, Libin Shi^b, Cuishi Guan^b, Dongyue Peng^b^,^*(), Shuhui Fang^a, Wei Zhang^a^,^c^,^d^,^*(), Yue Liu^a^,^c^,^*()

^a State Key Laboratory of Petroleum Molecular & Process Engineering, Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China
^b State Key Laboratory of Petroleum Molecular & Process Engineering, Sinopec Research Institute of Petroleum Processing Co., LTD., Beijing 100083, China
^c Engineering Center for Sustainable Carbon Science and Technology, East China Normal University, Shanghai 200241, China
^d Institute of Photochemistry and Photofunctional Materials, School of Materials and Chemistry, University of Shanghai for Science and Technology, Shanghai 200093, China

Received:2025-11-03 Accepted:2026-01-06 Online:2026-07-05 Published:2026-06-12
Supported by:
SINOPEC Research Institute of Petroleum Processing Co., Ltd(36800000-24-ZC0613-0023);National Natural Science Foundation of China(22472059);National Natural Science Foundation of China(22302069);National Natural Science Foundation of China(22309212);Natural Science Foundation of Shanghai(23ZR1418800);Science and Technology Commission of Shanghai(25520750100)

摘要/Abstract

摘要：

全球塑料年产量已超4亿吨, 但有效回收率不足10%, 大量塑料废弃物通过填埋、焚烧处理, 引发严重环境问题. 聚烯烃(聚乙烯(PE)、聚丙烯(PP))和聚苯乙烯(PS)占全球塑料产量的65%以上, 其惰性C-C骨架导致化学回收难度大. 传统热解技术需400 °C以上高温, 能耗大且产物选择性差; 机械回收存在严格分选、降级利用等局限, 难以处理混合塑料. 开发温和条件下高效、高选择性化学回收技术, 对实现塑料循环经济、缓解环境压力具有重要意义.

本文报道了一种基于GaCl₃的熔融盐路易斯酸催化体系(MgCl₂-4GaCl₃, 简称Mg-Ga), 在无溶剂、温和温度(≤ 170 °C)下实现了PE, PP, PS及其混合塑料的高效解聚. 该催化剂熔点低(~75 °C), 在反应温度下呈液态, 显著增强了催化剂与聚合物之间的传质和接触效率. 结果表明, 130 °C时 Mg-Ga催化剂可在30 min内实现PS的完全转化, PE与PP的转化率均超过60%. 通过与AlCl₃基催化剂对比, 发现GaCl₃在保持较强路易斯酸性的同时, 其低熔点的特性确保了反应体系处于液-固或液-液接触状态, 从而表现出更优异的催化活性, 说明催化剂相态对于催化活性至关重要. 而在PE/PS或PP/PS混合塑料反应中, PS解聚产生的芳香烃与聚烯烃C-C键断裂生成烯烃中间体, 在Mg-Ga催化下发生Friedel-Crafts烷基化反应, 形成烷基化芳烃, 不仅将混合塑料的总转化率提升至~85%, 而且使C₆-C₁₅芳烃中单环芳烃的选择性增至33.5%, 展现了显著的协同反应效应. 动力学研究表明, PP和PS在Mg-Ga催化下显示较低的表观活化能, 分别为42和76 kJ·mol^-1. 拉曼光谱表征揭示反应过程中Mg-Ga熔融盐形成了[GaCl₄]^-和[Ga₂Cl₇]^-等氯镓酸盐活性物种, 其中强路易斯酸性的[Ga₂Cl₇]^-可通过动态解离重组补充GaCl₃活性组分, 高效激活惰性C-C键. 最后, 考察了该催化体系对真实废塑料(如PE自封袋、PP离心管、PS泡沫等)及其混合塑料的适用性. 结果表明, 该催化体系对不同来源的真实塑料具有良好的降解活性, 在优化条件下塑料转化率均近90%, 液体产物收率约70%, 且产物分布可通过混合塑料比例灵活调控.

综上, 本工作开发了一种低温、无溶剂、高效的混合塑料化学回收新方法, 阐明了熔融盐催化剂通过强化相接触效率以提升解聚速率的核心机制, 耦合聚烯烃C-C键裂解与Friedel-Crafts烷基化反应调变产物分布, 为塑料循环利用与可持续发展提供了具有潜力的解决方案.

关键词: 聚烯烃, 聚苯乙烯, 熔融盐, 路易斯酸, 氯化镓, 解聚

Abstract:

The chemical recycling of polyolefins (PE, PP) and polystyrene (PS) remains a major challenge due to their chemical stability of C-C backbones as well as the limited accessibility of polymer chains to catalytic active sites. Here, we report a solvent-free, low-temperature, and synergistic depolymerization strategy using a GaCl₃-based molten Lewis acid catalyst for the efficient conversion of PE, PP, and PS, both individually and in mixed plastics streams. The low melting point of the catalyst ensures liquid-phase mobility and efficient contact between polymer and catalysts, achieving complete PS conversion and over 60% PE/PP conversion within 30 min. In mixed plastics, a synergistic reaction pathway mediated by carbocation-type intermediates enables Friedel-Crafts alkylation between PS-derived aromatics and polyolefin-derived olefins, enhancing overall conversion (~85%) and selectivity toward mono-alkylated aromatics (up to 33.5%). Raman spectra confirmed the formation of [GaCl₄]^- and [Ga₂Cl₇]^- chlorogallate species during the reaction. This study demonstrates a novel, integrated approach for solvent-free, selective, and energy-efficient chemical recycling of mixed plastics, highlighting GaCl₃-based molten salts as versatile catalysts for circular and sustainable plastic recycling.

Key words: Polyolefins, Polystyrene, Molten salt, Lewis acid, Plastic, Depolymerization

袁磊, 高志文, 石利斌, 管翠诗, 彭东岳, 方淑慧, 章伟, 刘玥. 温和条件下氯化镓基熔融盐催化聚烯烃与聚苯乙烯无溶剂化学回收[J]. 催化学报, 2026, 86: 137-148.

Lei Yuan, Zhiwen Gao, Libin Shi, Cuishi Guan, Dongyue Peng, Shuhui Fang, Wei Zhang, Yue Liu. Solvent-free chemical recycling of polyolefins and polystyrene under mild conditions via GaCl₃-based molten catalysts[J]. Chinese Journal of Catalysis, 2026, 86: 137-148.

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图/表 9

Fig. 1. Catalytic depolymerization of PE on different catalysts: phase distribution (a,d), carbon number selectivity (b,e), and product distribution in C4-15 (c,f) at 130 °C (a-c) and 100 °C (d-f). The break of y axis in (c) and (f) represents the selectivity from 50% to 75%. Reaction conditions: 1.0 g PE, 7.5 mmol MCl3 or 1.875 mmol MgCl2-MCl3 molten salts, 600 rpm, 15 min (M refers to Al or Ga).

Fig. 2. Catalytic depolymerization of PS on different catalysts: phase distribution (a,d), carbon number selectivity (b,e), and aromatic product distribution in C6-15 (c,f) at 130 °C (a-c) and 100 °C (d-f). Reaction conditions: 1.0 g PS, 7.5 mmol MCl3 or 1.875 mmol MgCl2-MCl3 molten salts, 600 rpm, 15 min. (M refers to Al or Ga).

Fig. 3. Correlation plot of ΔT1 (reaction temperature - catalyst melting point) and ΔT2 (reaction temperature - plastic melting point) for different conversion ranges in the reaction of PE or PS on AlCl3- and GaCl3-based catalysts. Circles represent the substrate PE (polyethylene), pentagons represent the substrate PS (polystyrene); solid symbols indicate the GaCl3-based catalyst, and semi-hollow symbols indicate the AlCl3-based catalyst.

Fig. 4. Time-resolved conversion of single-component polymer. Phase distribution PE (a), PP (b), and PS (c). Product distribution in PE (d), PP (e), and PS (f). GPC analysis of residual solid of PE (g), PP (h), and PS (i) after reaction. Reaction conditions: 1.0 g substrates, 1.875 mmol Mg-Ga, 130 °C, 600 rpm.

Fig. 5. Time-resolved conversion of PE-PS mixture (a-c) and PP-PS mixture (d-f), in terms of phase distribution (a,d), product distribution (b-c, e-f). Reaction conditions: 1.0 g substrates (mass ratio = 1:1), 1.875 mmol Mg-Ga, 130 °C, 600 rpm.

Scheme 1. Proposed reaction network exemplified by the PP-PS co-conversion over Mg-Ga catalyst.

Fig. 6. Initial conversion rates of PP (a) and PS (c) reaction catalyzed by Mg-Ga in the temperature range of 80-130 °C. Arrhenius plots for the initial conversion rate of PP (b) and PS (d). Ea in (b) and (d) refers to apparent activation energy. Reaction conditions: 1.0 g substrates, 1.875 mmol Mg-Ga, 600 rpm.

Fig. 7. Raman spectra of GaCl3-based catalysts. Reaction conditions: 1.0 g PE, 1.875 mmol Mg-Ga, 130 °C, 600 rpm, reaction time 1 min and 5 min.

Fig. 8. Catalytic depolymerization of post-consumer plastics on Mg-Ga. Reaction conditions: 1.0 g PE materials, 3.75 mmol Mg-Ga, 170 °C, 600 rpm, 12 h; 1.0 g PP/PS materials, 1.875 mmol Mg-Ga, 130 °C, 600 rpm, 12 h.

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温和条件下氯化镓基熔融盐催化聚烯烃与聚苯乙烯无溶剂化学回收

Solvent-free chemical recycling of polyolefins and polystyrene under mild conditions via GaCl₃-based molten catalysts

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温和条件下氯化镓基熔融盐催化聚烯烃与聚苯乙烯无溶剂化学回收

Solvent-free chemical recycling of polyolefins and polystyrene under mild conditions via GaCl3-based molten catalysts

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Solvent-free chemical recycling of polyolefins and polystyrene under mild conditions via GaCl₃-based molten catalysts