Yuan‐Fang Zhang

Abstract Soft robots have the appealing advantages of being highly flexible and adaptive to complex environments. However, the low‐stiffness nature of the constituent materials makes soft robotic systems incompetent in tasks requiring relatively high load capacity. Despite recent attempts to develop stiffness‐tunable soft actuators by employing variable stiffness materials and structures, the reported stiffness‐tunable actuators generally suffer from limitations including slow responses, small deformations, and difficulties in fabrication with microfeatures. This work presents a paradigm to design and manufacture fast‐response, stiffness‐tunable (FRST) soft actuators via hybrid multimaterial 3D printing. The integration of a shape memory polymer layer into the fully printed actuator body enhances its stiffness by up to 120 times without sacrificing flexibility and adaptivity. The printed Joule‐heating circuit and fluidic cooling microchannel enable fast heating and cooling rates and allow the FRST actuator to complete a softening–stiffening cycle within 32 s. Numerical simulations are used to optimize the load capacity and thermal rates. The high load capacity and shape adaptivity of the FRST actuator are finally demonstrated by a robotic gripper with three FRST actuators that can grasp and lift objects with arbitrary shapes and various weights spanning from less than 10 g to up to 1.5 kg.

Hydrogel-polymer hybrids have been widely used for various applications such as biomedical devices and flexible electronics. However, the current technologies constrain the geometries of hydrogel-polymer hybrid to laminates consisting of hydrogel with silicone rubbers. This greatly limits functionality and performance of hydrogel-polymer-based devices and machines. Here, we report a simple yet versatile multimaterial 3D printing approach to fabricate complex hybrid 3D structures consisting of highly stretchable and high-water content acrylamide-PEGDA (AP) hydrogels covalently bonded with diverse UV curable polymers. The hybrid structures are printed on a self-built DLP-based multimaterial 3D printer. We realize covalent bonding between AP hydrogel and other polymers through incomplete polymerization of AP hydrogel initiated by the water-soluble photoinitiator TPO nanoparticles. We demonstrate a few applications taking advantage of this approach. The proposed approach paves a new way to realize multifunctional soft devices and machines by bonding hydrogel with other polymers in 3D forms.

4D printing is an emerging fabrication technology that enables 3D printed structures to change configuration over "time" in response to an environmental stimulus. Compared with other soft active materials used for 4D printing, shape-memory polymers (SMPs) have higher stiffness, and are compatible with various 3D printing technologies. Among them, ultraviolet (UV)-curable SMPs are compatible with Digital Light Processing (DLP)-based 3D printing to fabricate SMP-based structures with complex geometry and high-resolution. However, UV-curable SMPs have limitations in terms of mechanical performance, which significantly constrains their application ranges. Here, a mechanically robust and UV-curable SMP system is reported, which is highly deformable, fatigue resistant, and compatible with DLP-based 3D printing, to fabricate high-resolution (up to 2 µm), highly complex 3D structures that exhibit large shape change (up to 1240%) upon heating. More importantly, the developed SMP system exhibits excellent fatigue resistance and can be repeatedly loaded more than 10 000 times. The development of the mechanically robust and UV-curable SMPs significantly improves the mechanical performance of the SMP-based 4D printing structures, which allows them to be applied to engineering applications such as aerospace, smart furniture, and soft robots.

Abstract Four-dimensional (4D) printing of shape memory polymer (SMP) imparts time responsive properties to 3D structures. Here, we explore 4D printing of a SMP in the submicron length scale, extending its applications to nanophononics. We report a new SMP photoresist based on Vero Clear achieving print features at a resolution of ~300 nm half pitch using two-photon polymerization lithography (TPL). Prints consisting of grids with size-tunable multi-colours enabled the study of shape memory effects to achieve large visual shifts through nanoscale structure deformation. As the nanostructures are flattened, the colours and printed information become invisible. Remarkably, the shape memory effect recovers the original surface morphology of the nanostructures along with its structural colour within seconds of heating above its glass transition temperature. The high-resolution printing and excellent reversibility in both microtopography and optical properties promises a platform for temperature-sensitive labels, information hiding for anti-counterfeiting, and tunable photonic devices.

Abstract Flexible transparent electrodes (FTEs) with embedded metal meshes play an indispensable role in many optoelectronic devices due to their excellent mechanical stability and environmental adaptability. However, low‐cost, simple, efficient, and environmental friendly integrated manufacturing of high‐performance embedded metal meshes remains a huge challenge. Here, a facile and novel fabrication method is proposed for FTEs with an embedded metal mesh via liquid substrateelectric‐field‐driven microscale 3D printing process. This direct printing strategy avoids tedious processes and offers low‐cost and high‐volume production, enabling the fabrication of high‐resolution, high‐aspect ratio embedded metal meshes without sacrificing transparency. The final manufactured FTEs with 80 mm × 80 mm embedded metal mesh offers excellent optoelectronic performance with a sheet resistance ( R s ) of 6 Ω sq −1 and a transmittance ( T ) of 85.79%. The embedded metal structure still has excellent mechanical stability and good environmental suitability under different harsh working conditions. The practical feasibility of the FTEs is successfully demonstrated with a thermally driven 4D printing structure and a resistive transparent strain sensor. This method can be used to manufacture large areas with facile, high‐efficiency, low‐cost, and high‐performance FTEs.