Light-Controlled Triple-Shape-Memory, High-Permittivity Dynamic Elastomer for Wearable Multifunctional Information Encoding Devices.

Self-powered information encoding devices (IEDs) have drawn considerable interest owing to their capability to process information without batteries. Next-generation IEDs should be reprogrammable, self-healing, and wearable to satisfy the emerging requirements for multifunctional IEDs; however, such devices have not been demonstrated. Herein, an integrated triboelectric nanogenerator-based IED with the aforementioned features was developed based on the designed light-responsive high-permittivity poly(sebacoyl diglyceride-co-4,4'-azodibenzoyl diglyceride) elastomer (PSeDAE) with a triple-shape-memory effect. The electrical memory feature was achieved through a microscale shape-memory property, enabling spatiotemporal information reprogramming for the IED. Macroscale shape-memory behavior afforded the IED shape-reprogramming ability, yielding wearable and detachable features. The dynamic transesterifications and light-heating groups in the PSeDAE afforded a remotely controlled rearrangement of its cross-linking network, producing the self-healing IED.

Self-healing polyurethane-elastomer with mechanical tunability for multiple biomedical applications in vivo.

The unique properties of self-healing materials hold great potential in the field of biomedical engineering. Although previous studies have focused on the design and synthesis of self-healing materials, their application in in vivo settings remains limited. Here, we design a series of biodegradable and biocompatible self-healing elastomers (SHEs) with tunable mechanical properties, and apply them to various disease models in vivo, in order to test their reparative potential in multiple tissues and at physiological conditions. We validate the effectiveness of SHEs as promising therapies for aortic aneurysm, nerve coaptation and bone immobilization in three animal models. The data presented here support the translation potential of SHEs in diverse settings, and pave the way for the development of self-healing materials in clinical contexts.

3D printing preview for stereo-lithography based on photopolymerization kinetic models.

The diversity of biomedical applications makes stereolithographic (SL) three-dimensional (3D) printing process complex. A strategy was developed to simulate the layer-by-layer fabrication of 3D printed products combining polymerization kinetic with reaction conditions to realize print preview. As a representative example, the typical UV-curable dental materials based on epoxy acrylate and photoinitiator with different molar ratios was exposed under varying intensity of UV light to verify the simulation results. A theoretical kinetics model containing oxygen inhibition was established. In-situ FTIR was employed to measure propagation and termination constants while coupled UV/vis was performed to examine the law of light attenuation during cure reaction, even with various colours and additives. Simulation results showed that the correlation coefficient square between the experiments and simulations of epoxy acrylate with 1%, 2% and 3% initiator upon 20 mW/cm2 UV light are 0.8959, 0.9324 and 0.9337, respectively. Consequently, our simulation of photopolymerization for SL 3D printing successfully realized visualization of printing quality before practically printing the targeted biomedical objects with complex topology structures.

Biofunctionalized chondrogenic shape-memory ternary scaffolds for efficient cell-free cartilage regeneration.

Cartilage defect repair remains a great clinical challenge due to the limited self-regeneration capacity of cartilage tissue. Surgical treatment of injured cartilage is rather difficult due to the narrow space in the articular cavity and irregular defect area. Herein, we designed and fabricated chondrogenic and physiological-temperature-triggered shape-memory ternary scaffolds for cell-free cartilage repair, where the poly (glycerol sebacate) (PGS) networks ensured elasticity and shape recovery, crystallized poly (1,3-propylene sebacate) (PPS) acted as switchable phase, and immobilized bioactive kartogenin (KGN) endowed the scaffolds with chondrogenic capacity. The resultant scaffolds exhibited shape-memory properties with shape-memory fixed ratio of 98% and recovered ratio of 97% at 37°C for PPS/PGS/KGN-100, indicating a good potential for minimally invasive implantation. The scaffolds gradually degraded in Dulbecco's phosphate-buffered saline and released KGN up to 12 weeks in vitro. In addition, the scaffolds promoted chondrogenic differentiation while inhibiting osteogenic differentiation of bone marrow-derived mesenchymal stem cells in a concentration-dependent manner and cartilage regeneration in full-thickness defects of rat femoropatellar groove for 12 weeks. Consequently, the PPS/PGS/KGN-100 scaffolds stimulated the formation of an overlying layer of neocartilage mimicking the characteristic architecture of native articular cartilage even in the absence of exogenous growth factors and seeded cells. This study provides much inspiration for future research on cartilage tissue engineering. STATEMENT OF SIGNIFICANCE: There are two crucial challenges for cartilage defect repair: the lack of self-regeneration capacity of cartilage tissue and difficult scaffold implantation via traditional open surgery due to space-limited joints. Herein, bioactive body-temperature-responsive shape memory scaffolds are designed to simultaneously address the challenges. The scaffolds can be readily implanted by minimally invasive approach and recover by body-temperature of patient. The integration of kartogenin endows scaffolds the bioactivity, leading to the first example of bulk shape-memory scaffolds for cell-free cartilage repair. These characteristics make the scaffolds advantageous for clinical translation. Moreover, our developed material is easy to be functionalized due to the presence of extensive free hydroxyl groups and provides a versatile platform to design diverse functional shape memory biomaterials.

Mechanically and biologically skin-like elastomers for bio-integrated electronics.

The bio-integrated electronics industry is booming and becoming more integrated with biological tissues. To successfully integrate with the soft tissues of the body (eg. skin), the material must possess many of the same properties including compliance, toughness, elasticity, and tear resistance. In this work, we prepare mechanically and biologically skin-like materials (PSeD-U elastomers) by designing a unique physical and covalent hybrid crosslinking structure. The introduction of an optimal amount of hydrogen bonds significantly strengthens the resultant elastomers with 11 times the toughness and 3 times the strength of covalent crosslinked PSeD elastomers, while maintaining a low modulus. Besides, the PSeD-U elastomers show nonlinear mechanical behavior similar to skins. Furthermore, PSeD-U elastomers demonstrate the cytocompatibility and biodegradability to achieve better integration with tissues. Finally, piezocapacitive pressure sensors are fabricated with high pressure sensitivity and rapid response to demonstrate the potential use of PSeD-U elastomers in bio-integrated electronics.