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A water-recyclable; robust; and self-healing sugar-based supramolecular network enabled by Maillard-analogous initialization of polymerization
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DOI：10.1039/D5MH01828E.png)
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Abstract
En 中文
Crosslinked functional polymers exhibit exceptional mechanical and chemical properties critical for applications spanning biomedical engineering; advanced adhesives; and self-healing materials. However; challenges in recycling; either due to irreversible crosslinks or; in the case of covalent adaptable networks (CANs); limited solid-state plasticity that typically requires catalysts; significantly restrict sustainability. To address these limitations; we present a novel water-mediated polymerization strategy inspired by the radical-generating mechanism of the Maillard reaction; utilizing maltose as both an initiator and a functional side group in a simple; catalyst-free; aqueous reaction with acrylamide (AAm). This mild; one-pot reaction occurs below 100 °C; forming adaptively functionalized supramolecular networks (AFSNs) that form supramolecular networks through hydrogen bonding and display dynamic imine linkages to the maltose side chains supporting self-healing and re-shaping. These elastomers are characterized by impressive mechanical strength (up to 5 MPa tensile strength); high elongation (up to 1000%); notable fracture energy (36 kJ m−2); robust adhesive performance (up to 4.8 MPa); and rapid self-healing capability at room temperature. Crucially; the elastomer's supramolecular network can be fully and repeatedly dissolved and reprocessed using only water; preserving mechanical integrity without chemical degradation. This sustainable approach provides a practical solution for synthesizing and recycling high-performance crosslinked materials while eliminating environmental hazards; guiding the future development of green polymer chemistry and functional material design.
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