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Supramolecular Ionic Polymerization: Cellulose-Based Supramolecular Plastics with Broadly Tunable Mechanical Properties

Journal of the American Chemical Society 2025 1 citation ? Citation count from OpenAlex, updated daily. May differ slightly from the publisher's own count. Score: 53 ? 0–100 AI score estimating relevance to the microplastics field. Papers below 30 are filtered from public browse.
Zhenghong Chen, Hong Yang, Hiroyuki Inuzuka, Kiichi Mizukami, Takuzo Aida

Summary

Researchers developed a cellulose-based supramolecular plastic by combining carboxymethyl cellulose with a hyperbranched polyguanidinium ion through ionic bonding. The resulting material demonstrated broadly tunable mechanical properties including high strength and stretchability comparable to conventional petroleum-based plastics. The study presents a promising approach for creating sustainable, biodegradable plastic alternatives from renewable biomass resources that could help reduce microplastic pollution.

Study Type Environmental

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.

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