Polyolefins, such as HDPE, LDPE, and PP, comprise the largest volume of commodity plastics, but their recycling is hampered by their chemical inertness, which does not allow easy functionalization or depolymerization back to monomer. For example, thermolysis of HDPE promotes random chain scission of carbon-carbon bonds to yield little monomer but mostly waxes with various molecular weights and gasoline liquids (C4-C9 products). These products might be useful as fuels but provide little value as building blocks for functional materials. In this work, we develop a new method for controlled chain cleavage of polyolefins, such as HDPE, to generate telechelic waxes (e.g. C100-C1000 products with functional end groups) that can be used as raw materials for fabricating a variety of value-added functional materials. This materials development platform for polyolefin upcycling is based on controlled breakdown of polyethylene chains through a scalable, three-step process that produces short chain oligomers with functional and reactive end-groups, such as alcohol, acrylate, etc. Each step was developed and optimized using a model long-chain alkane compound, octacosane, and an array of spectroscopic and spectrometric characterization methods. Successful application of this method to virgin high-density polyethylene was also demonstrated.

Polyethylene upcycling through controlled breakdown and functionalization

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ACS Fall 2022

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