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Two-way reversible shape memory polymers (2W-SMPs) are highly desirable for many applications. We report for the first time the use of random copolymers with cocrystallizable monomeric units for the preparation of such polymer networks. Homopolymers and random copolymers of ε-caprolactone and ω-pentadecalactone were designed and made by ring-opening polymerization with Candida antarctica lipase B as catalyst. The melting temperatures of these prepolymers may be adjusted by the use of various molar ratios of the comonomers. Upon thiol–ene cross-linking, the polymer network exhibited two-way reversible shape memory effects under both stress-free and stress conditions. The actuation temperature (T A) of the 2W-SMP under stress-free condition can be tuned in a broad range using a selected mixture of prepolymers followed by photo-cross-linking with a multifunctional cross-linker. Increasing the initial stretching stress amplitude led to an increased absolute strain change under both stress-free and stress condition; it led to a reduced relative strain change under stress-free condition, but almost no change under stress condition. The evolution of the microstructure of 2W-SMPs under stress-free condition cycle was studied by the use of X-ray diffraction (2D-WAXD and SAXS). This is the first report on the tuning of T A of 2W-SMPs under stress-free condition by the use of one or two prepolymers to form a chemically cross-linked network. We have also eliminated the use of toxic metal catalysts in the synthesis of polymeric biomaterials. The materials are shown to be capable of performing reversible bending–unbending and coiling–uncoiling motions.

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This review presents the recent developments in the research hotspots of advanced functional polymers; their concepts, design strategies, and applications are briefly discussed.

Two-way reversible shape memory polymers (2W-SMPs), especially those that are light-responsive, are highly desirable for many applications, especially in the biomedical field, because of the convenience of indirect heating. We have designed and prepared a series of light-actuated 2W-SMP composites by incorporating very small amounts of polydopamine (PDA) nanospheres into semicrystalline polymer networks based on biodegradable poly­(ε-caprolactone) copolymers. PDA nanospheres can be well dispersed in chloroform and well mixed with the polymer network. PDA nanospheres manifest good photothermal effect because of their strong absorption of light. The variation in temperature of the polymer composites can be correlated with irradiation time, light intensity, and the content of PDA nanospheres. Equations are developed to fit the temperature changes of the materials as a function of irradiation power and of the PDA particles content for a better understanding of the kinetics of the light-to-heat conversion. These polymer composites show excellent two-way reversible shape memory effects (2W-SMEs) under stress-free condition when the light is switched on and off showing a reversible angle change of 45°. The speed of angle change is larger for polymer composites irradiated with a stronger light or with a higher content of PDA nanospheres. This is the first report on 2W-SMPs using incorporated PDA nanospheres as photothermal fillers. A moving robot is designed based on photoresponsive 2W-SMP composites, which can walk on a track with triangular saw-teeth. This composite is capable of lifting and lowering a weight, acting as artificial muscles, and its actuated stress is much higher than the maximum stress yielded by most mammalian skeletal muscles. The use of biodegradable polyesters and thermal fillers made of a natural compound dopamine makes such composites potentially useful as biomaterials.