TY - JOUR A1 - Fong, Mun‐Oon A1 - Chen, Xiangping A1 - Wong, Jie‐Wei A1 - Lok, Tow‐Jie A1 - Li, Siyang A1 - Low, Jia Tee A1 - Nordin, Nur Syahirra A1 - Miao, Zhikun A1 - Hu, Qiannan A1 - Neffe, Axel T. A1 - Wong, Tuck‐Whye A1 - Li, Tiefeng A1 - Yang, Wei T1 - Multifunctional Roles of Iron Oxide Nanoparticles in a Reversible Shape‐Memory Composite JF - Advanced Functional Materials N2 - The utilization of functional fillers in the development of composite materials has come a long way since its advent to improve physical, chemical, or mechanical properties of the base material. However, the heterogenous roles contributed by a single type of filler remain uncommon in this field. Here the endowment of various modifications to a 1,8‐octanediol/1,12‐dodecanedioic acid/citric acid (OD/DDA/CA) matrix through the incorporation of iron oxide nanoparticles (IONPs) is reported. Owing to the relaxation and hysteresis loss behaviors of IONPs when exposed to an alternating magnetic field (AMF), the composites demonstrate a magnetothermal response. Similarly, the excitation and relaxation of electrons in IONPs under near‐infrared light (NIR) enable photothermic‐responsiveness. In combination, two findings nurtured an observed shape‐memory effect when the samples are under actuation by these indirect stimuli, where a shape recovery ratio (≥98%) and reversible strain (≤7%) are recorded. Moreover, the catalytic role of IONPs aided transesterification in the covalent network, demonstrated by successful repeated cycles of shape reconfiguration of the samples. This work highlights the prospectives of multifunctional composite fillers in the exploration of bio‐derived composite smart materials. KW - Shape-Memory Polymer KW - Composite KW - Iron Oxide Nanoparticle KW - bio-based Y1 - 2024 U6 - https://doi.org/10.1002/adfm.202418409 SN - 1616-301X PB - Wiley ER - TY - GEN A1 - Li, Siyang A1 - Lok, Tow-Jie A1 - Ngo, Shi-Han A1 - Xue, Yaoting A1 - Miao, Zhikun A1 - Feng, Tao A1 - Wang, Lei A1 - Wong, Jie-Wei A1 - Low, Jiatee A1 - Lim, Kai-Yi A1 - Woon, Min-Rou A1 - Neffe, Axel T. A1 - Wong, Tuck-Whye A1 - Li, Tiefeng A1 - Yang, Xuxu A1 - Yang, Wei T1 - A water-recyclable, robust, and self-healing sugar-based supramolecular network enabled by Maillard-analogous initialization of polymerization T2 - Materials horizons N2 - 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. KW - Recycling KW - biobased polymer KW - self-healing KW - Maillard Y1 - 2026 U6 - https://doi.org/10.1039/D5MH01828E SN - 2051-6347 VL - 13 IS - 1 SP - 219 EP - 232 PB - Royal Society of Chemistry (RSC) CY - Cambridge ER -