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开发高性能且可持续的聚乳酸/回收聚烯烃共混物:调节官能团反应程度与性能优化。

Developing high-performance and sustainable polylactic acid/recycled polyolefin blends: Tuning the degree of functional group reaction and performance optimization.

作者信息

Yu Lingxiao, Qiu Ying, Yang Bing, Gao Meng, Song Lixin, Jing Ying, Chi Weihan, Wang Xiangyi, Zhang Liwu, Gao Jialu, Huang Jiangting, Li Yongchao, Gao Guangxu, Gao Yujuan, Wang Yuanxia, Wang Na

机构信息

Liaoning Provincial Key Laboratory for Synthesis and Preparation of Special Functional Materials, Shenyang University of Chemical Technology, Shenyang 110142, Liaoning, China; College of Materials Science and Engineering, Shenyang University of Chemical Technology, Shenyang 110142, China.

College of Chemistry, Jilin University, Changchun 130012, China.

出版信息

Int J Biol Macromol. 2025 Feb;289:138554. doi: 10.1016/j.ijbiomac.2024.138554. Epub 2024 Dec 7.

Abstract

In the current development of the plastics industry, the use of biodegradable and recycled plastics not only effectively reduces the volume of landfills and incineration but also significantly decreases environmental damage. However, the extensive application of biodegradable polylactic acid (PLA) is limited by its poor toughness and thermal properties. The study introduced recycled linear low-density polyethylene (R-LLDPE) and ethylene-octene copolymer (POE) to modify PLA, primarily based on their excellent toughness and thermal resistance. Furthermore, being a recycled material, R-LLDPE is economically advantageous and conforms to the ecological requirements of resource recycling. Therefore,the study introduced glycidyl methacrylate (GMA) and styrene (St) to synthesize the graft copolymer (R-LLDPE/POE)-g-(GMA-co-St) (RPGS). The RPGS serves as a modifier for PLA resin. The effects of different GMA amounts in RPGS on the properties and microstructure of PLA/RPGS blends were examined. The results illustrate that GMA was successfully grafted onto the molecular chains of R-LLDPE/POE (RP), with St acting as a "bridge" to enhance further the grafting efficiency of GMA on RP macromolecular chains. After introducing RPGS into the PLA matrix, the epoxy groups of GMA reacted with the terminal hydroxyl groups of PLA, significantly decreasing the particle size of the dispersed phase and closely integrating with the PLA matrix, hence greatly improving the compatibility between PLA and RP. With the increase of GMA amount, the optical, thermal, and hydrophobic properties of the blends were increased, while the flexibility first increased and then decreased. When the amount of GMA was 5 wt% in RPGS, the G and G of GMA reached optimal values of 2.55 % and 51 %, the blend exhibited the optimum overall properties: haze decreased to 28.3 %, light transmittance increased to 92.5 %, thermal decomposition temperature increased to 368.12 °C, and the Vicat softening temperature increased to 78.2 °C. While maintaining the tensile strength at 54.3 MPa, the notched impact strength and elongation at break increased to 10,182.4 J/m and 231.7 %, respectively, with the matrix exhibiting significant shear yielding. The research presents an eco-friendly and efficient method for producing high-performance PLA-based materials, effectively addressing the shortcomings of PLA in toughness and thermal resistance. The modified materials had excellent mechanical and thermal capabilities while offering financial and environmental benefits. The development of this material is anticipated to enhance the industrial utilization of biodegradable and recycled plastics, offering essential support for attaining sustainable manufacturing and a circular economy.

摘要

在当前塑料工业的发展中,使用可生物降解和回收塑料不仅能有效减少填埋和焚烧的体积,还能显著降低对环境的破坏。然而,可生物降解聚乳酸(PLA)的广泛应用受到其较差的韧性和热性能的限制。该研究引入回收线性低密度聚乙烯(R-LLDPE)和乙烯-辛烯共聚物(POE)来改性PLA,主要基于它们优异的韧性和耐热性。此外,作为一种回收材料,R-LLDPE具有经济优势,符合资源回收的生态要求。因此,该研究引入甲基丙烯酸缩水甘油酯(GMA)和苯乙烯(St)合成接枝共聚物(R-LLDPE/POE)-g-(GMA-co-St)(RPGS)。RPGS用作PLA树脂的改性剂。研究了RPGS中不同GMA用量对PLA/RPGS共混物性能和微观结构的影响。结果表明,GMA成功接枝到R-LLDPE/POE(RP)的分子链上,St作为“桥梁”进一步提高了GMA在RP大分子链上的接枝效率。将RPGS引入PLA基体后,GMA的环氧基团与PLA的端羟基反应,显著减小了分散相的粒径,并与PLA基体紧密结合,从而大大提高了PLA与RP之间的相容性。随着GMA用量的增加,共混物的光学、热学和疏水性能增强,而柔韧性先增加后降低。当RPGS中GMA的用量为5 wt%时,GMA的接枝率和接枝效率分别达到最佳值2.55%和51%,共混物表现出最佳的综合性能:雾度降至28.3%,透光率提高到92.5%,热分解温度提高到368.12℃,维卡软化温度提高到78.2℃。在保持拉伸强度为54.3 MPa的同时,缺口冲击强度和断裂伸长率分别提高到10182.4 J/m和231.7%,基体呈现出明显的剪切屈服。该研究提出了一种生产高性能PLA基材料的环保高效方法,有效解决了PLA在韧性和耐热性方面的不足。改性材料具有优异的机械和热性能,同时具有经济和环境效益。这种材料的开发有望提高可生物降解和回收塑料的工业利用率,为实现可持续制造和循环经济提供重要支持。

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