Nature excels in both self-healing and 3D shaping; for example, self-healable human organs feature functional geometries and microstructures. However, tailoring man-made self-healing materials into complex structures faces substantial challenges. Here, we report a paradigm of photopolymerization-based additive manufacturing of selfhealable elastomer structures with free-form architectures. The paradigm relies on a molecularly designed photoelastomer ink with both thiol and disulfide groups, where the former facilitates a thiol-ene photopolymerization during the additive manufacturing process and the latter enables a disulfide metathesis reaction during the selfhealing process. We find that the competition between the thiol and disulfide groups governs the photocuring rate and self-healing efficiency of the photoelastomer. The self-healing behavior of the photoelastomer is understood with a theoretical model that agrees well with the experimental results. With projection microstereolithography systems, we demonstrate rapid additive manufacturing of single-and multimaterial self-healable structures for 3D soft actuators, multiphase composites, and architected electronics. Compatible with various photopolymerization-based additive manufacturing systems, the photoelastomer is expected to open promising avenues for fabricating structures where free-form architectures and efficient self-healing are both desirable.

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The development of thermal conductive polymer composite is necessary for the application in thermal management. In this paper, the experimental and theoretical investigations have been conducted to determine the effect of copper nanowires (CuNWs) and copper nanoparticles (CuNPs) on the thermal conductivity of dimethicone nanocomposites. The CuNWs and CuNPs were prepared by using a liquid phase reduction method, and they were characterized through scanning electron microscopy (SEM) and X-ray diffraction (XRD). The experimental data show that the thermal conductivity of composites increases with the increase of filler. With the addition of 10 vol.% CuNWs, the thermal conductivity of the composite is 0.41 W/m/K. The normalized thermal conductivity enhancement factor is 2.73, much higher than that of the analogue containing CuNPs (1.67). These experimental data are in agreement with Nan’s model prediction. Due to the high aspect ratio of 1D CuNWs, they can construct thermal networks more effectively than CuNPs in the composite, resulting in higher thermal conductivity.

Emerging transformable lattice structures provide promising paradigms to reversibly switch lattice configurations, thereby enabling their properties to be tuned on demand. The existing transformation mechanisms are limited to nonfracture deformation, such as origami, instability, shape memory, and liquid crystallinity. In this study, we present a class of transformable lattice structures enabled by fracture and shape-memory-assisted healing. The lattice structures are additively manufactured with a molecularly designed photopolymer capable of both fracture healing and shape memory. We show that 3D-architected lattice structures with various volume fractions can heal fractures and fully restore stiffness and strength over two to ten healing cycles. In addition, coupled with the shape-memory effect, the lattice structures can recover fracture-associated distortion and then heal fracture interfaces, thereby enabling healing of lattice wing damages, mode-I fractures, dent-induced crashes, and foreign-object impacts. Moreover, by harnessing the coupling of fracture and shape-memory-assisted healing, we demonstrate reversible configuration transformations of lattice structures to enable switching among property states of different stiffnesses, vibration transmittances, and acoustic absorptions. These healable, memorizable, and transformable lattice structures may find broad applications in next-generation aircraft panels, automobile frames, body armor, impact mitigators, vibration dampers, and acoustic modulators.