The green revolution in plastics should be accelerated due to growing sustainability concerns. Here, we develop a series of chemically recyclable polymers from the first reported cascade polymerization of H2O, COS, and diacrylates. In addition to abundant feedstocks, the method is efficient and air‐tolerant, uses common organic bases as catalysts, and yields polymers with high molecular weights under mild conditions. Such polymers, structurally like polyethylene with low‐density in‐chain polar groups, manifest impressive toughness and ductility comparable to high‐density polyethylene. The in‐chain ester group acts as a breaking point, enabling these polymers to undergo chemical recycling through two loops. The structures and properties of these polymers also have an immeasurably expanded range owing to the versatility of our method. The readily available raw materials, facile synthesis, and high performance make these polymers promising prospects as sustainable materials in practice.

Five-membered cyclic carbonate (5-CC) has the advantages of wide availability, low toxicity, and low volatility, but extremely low ring strain makes it a thermodynamically "non-polymerizable" monomer. This work, for the...

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The facile synthesis of chemically recyclable polymers derived from sustainable feedstocks presents enormous challenges. Here, we develop a novel, modular, and efficient click reaction for connecting primary, secondary, or tertiary alcohols with activated alkenes via a bridge molecule of carbonyl sulfide (COS). The click reaction is successfully applied to synthesize a series of recyclable polymers by the step polyaddition of diols, diacrylates, and COS. Diols and diacrylates are common chemicals and can be produced from biorenewable sources, and COS is released as the industrial waste. In addition to sustainable monomers, the approach is atom‐economical, wide in scope, metal‐free, and performed under mild conditions, affording unprecedented polymers with nearly quantitative yields. The produced polymers also possess predesigned and widely tunable structure owing to the versatility of our method and the broad variety of monomers. The in‐chain thiocarbonate and ester polar groups can play as breakpoints, allowing these polymers to be easily recycled. Overall, the polymers have broad prospects for green materials given their facile synthesis, readily available feedstocks, desirable performance, and chemical recyclability.

The green revolution in plastics should be accelerated due to growing sustainability concerns. Here, we develop a series of chemically recyclable polymers from the first reported cascade polymerization of H2O, COS, and diacrylates. In addition to abundant feedstocks, the method is efficient and air‐tolerant, uses common organic bases as catalysts, and yields polymers with high molecular weights under mild conditions. Such polymers, structurally like polyethylene with low‐density in‐chain polar groups, manifest impressive toughness and ductility comparable to high‐density polyethylene. The in‐chain ester group acts as a breaking point, enabling these polymers to undergo chemical recycling through two loops. The structures and properties of these polymers also have an immeasurably expanded range owing to the versatility of our method. The readily available raw materials, facile synthesis, and high performance make these polymers promising prospects as sustainable materials in practice.