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Supramolecular IonicPolymerization: Cellulose-BasedSupramolecular Plastics with Broadly Tunable Mechanical Properties
Summary
Researchers created a cellulose-based supramolecular plastic via ionic polymerization and showed that mechanical brittleness could be overcome with choline chloride addition, yielding a renewable, tunable material as a potential microplastic-free alternative to petroleum-based plastics.
Developing mechanically tough and sustainable plastics from renewable resources such as biomass may certainly give a promising solution to the replacement of petroleum-based plastics and eliminate microplastics. Here, we report a cellulose-based supramolecular plastic (CMCSP) synthesized by supramolecular “ionic” polymerization of carboxymethyl cellulose (CMC) as an oxyanionic monomer and a hyperbranched polyguanidinium ion (PEIGu) as a cationic monomer. CMCSP is mechanically strong but inherently brittle. However, as highlighted in the present paper, we could overcome the brittleness issue by adding (2-hydroxyethyl)trimethylammonium chloride (choline chloride, ChCl) to CMCSP. This FDA-approved, biodegradable ionic human nutrient served as a particular plasticizer, enabling broad modulation of stiff, glassy CMCSP to a tough, flexible material and further to a soft, elastic material. We demonstrated that plasticized CMCSPChCl could be processed into a flexible plastic bag, which was mechanically tough but perfectly dissociable in seawater and closed-loop recyclable with electrolytes. Hence, CMCSPChCl never generates microplastics.