LEGO's Strategy to Upcycle Waste Polyethylene into High-Performance Materials

Sichuan University Wang Yuzhong An academician team has proposed an innovative "Lego" strategy to successfully upgrade and recycle waste polyethylene (PE) into multifunctional high-performance materials. This strategy involves degrading PE into oligomers, which are then assembled with different functional monomer modules through dynamic imine bonds.
This allows for customized functionalization, achieving multiple functions such as flame retardancy, antistatic properties, UV protection, and colorability. At the same time, the resulting materials exhibit good physical and chemical recyclability. This article was published as an open-access research article in the flagship journal of the Chinese Chemical Society, "CCS ChemistryUp.
Creating multifunctional materials with dynamic covalent networks.
Polyethylene (PE), as one of the most widely produced and utilized plastics, presents challenges in functionalization and chemical degradation due to its chemical inertness. Simultaneously, the growing environmental pressure from the large volume of waste PE is increasingly concerning.
Traditional methods for functionalizing polyethylene (PE) often rely on physical blending, copolymerization with polar monomers, or chemical grafting. These approaches frequently encounter problems such as poor compatibility, synthetic difficulties, limited functionality, or compromised mechanical properties. Achieving high-value and multi-functional recycling of PE is a significant challenge currently facing the plastics circular economy.
To solve the aforementioned problems, Sichuan UniversityWang Yuzhong An academician team proposed the "LEGO" strategy, which involves a two-step process for PE upgrading and recycling. First, PE is controlled to form oligomers with active end groups (ADOPE-CHO), and then it is chemically reconstructed with various functional modules (such as flame retardant/UV shielding modules and antistatic/dyeable modules) through dynamic imine bonds to construct multifunctional materials with dynamic cross-linked networks.
The peak heat release rate was reduced by 73% compared to the original PE.
This dynamically cross-linked multi-functional material exhibits excellent mechanical properties and solvent resistance. Its tensile strength can reach 27 MPa, almost four times that of original PE. Meanwhile, it shows low swelling and mass loss rates in most solvents.
This flame retardant/UV resistant material exhibits a limiting oxygen index of up to 27%, enabling self-extinguishment in air. The peak heat release rate is reduced by up to 73% compared to virgin PE. The formation of flammable small olefin molecules is significantly suppressed during thermal decomposition, and the charring ability is significantly enhanced, achieving a residual mass of up to 33% at 700°C. A stable char layer can form during combustion, providing thermal and oxygen insulation. Furthermore, this material achieves full-band UV shielding.
The surface and volume resistivities of the obtained antistatic/dyeable material were reduced by 2-3 orders of magnitude compared to original PE, meeting the standard for static dissipative materials. The material can be dyed deep blue with methylene blue solution, exhibiting good color fastness, with no dye bleeding. Different colors can be achieved by adjusting the concentration or type of the dye solution.
Due to the inherent lack of reactive functional groups in PE, its functionalization is typically achieved through blending with functional fillers, which leads to significant polarity differences, poor compatibility, and decreased mechanical properties after blending modification. This degradable dynamic crosslinking reconstruction method not only enables modular construction of multifunctional materials but also significantly enhances the mechanical properties of the materials.
Based on the dynamic nature of imine bonds under thermal stimulation and their ability to dissociate in acidic organic solutions, materials can be physically recycled through multiple thermal processes or chemically recovered through complete degradation under acidic conditions.
Abstract and Outlook
In summary, this work adopts a "Lego" strategy to transform waste PE into high-performance, multi-functional, and recyclable new materials, achieving a recycling process that upgrades "waste plastics" into "high-value materials." This strategy boasts high flexibility, allowing for further functionalization based on specific needs, and provides new insights for the functional modification and high-value recycling of polyolefin plastics.
The study was recently published in the [Journal Name]. CCS Chemistrypublished in the journal "==". Shen Chengfeng, a doctoral student at Sichuan University, is the first author of this article, and Professor Xu Shimei and Wang Yuzhong The academician is the corresponding author. This research was supported by the National Natural Science Foundation of China.
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