Magnetically Actuated Trigger Transient Soft Actuators Comprising On-Demand Photo-Initiated and Thermo-Degradable Polypropylene Carbonate-Photo-Acid Generator.

Lifetime-reconfigurable soft robots have emerged as a new class of robots, emphasizing the unmet needs of futuristic sustainability and security. Trigger-transient materials that can both actuate and degrade on-demand are crucial for achieving life-reconfigurable soft robots. Here, we propose the use of transient and magnetically actuating materials that can decompose under ultraviolet light and heat, achieved by adding photo-acid generator (PAG) and magnetic particles (Sr-ferrite) to poly(propylene carbonate) (PPC). Chemical and thermal analyses reveal that the mechanism of PPC-PAG decomposition occurs through PPC backbone cleavage by the photo-induced acid. The self-assembled monolayer (SAM) encapsulation of Sr-ferrite preventing the interaction with the PAG allowed the transience of magnetic soft actuators. We demonstrate remotely controllable and degradable magnetic soft kirigami actuators using blocks with various magnetized directions. This study proposes novel approaches for fabricating lifetime-configurable magnetic soft actuators applicable to diverse environments and applications, such as enclosed/sealed spaces and security/military devices.

Lifetime-configurable soft robots via photodegradable silicone elastomer composites.

Developing soft robots that can control their own life cycle and degrade on-demand while maintaining hyperelasticity is a notable research challenge. On-demand degradable soft robots, which conserve their original functionality during operation and rapidly degrade under specific external stimulation, present the opportunity to self-direct the disappearance of temporary robots. This study proposes soft robots and materials that exhibit excellent mechanical stretchability and can degrade under ultraviolet light by mixing a fluoride-generating diphenyliodonium hexafluorophosphate with a silicone resin. Spectroscopic analysis revealed the mechanism of Si─O─Si backbone cleavage using fluoride ion (F-) and thermal analysis indicated accelerated decomposition at elevated temperatures. In addition, we demonstrated a robotics application by fabricating electronics integrated gaiting robot and a fully closed-loop trigger disintegration robot for autonomous, application-oriented functionalities. This study provides a simple yet novel strategy for designing life cycle mimicking soft robotics that can be applied to reduce soft robotics waste, explore hazardous areas, and ensure hardware security with on-demand destructive material platforms.

Fast and Durable Nanofiber Mat Channel Organic Electrochemical Transistors.

Bioelectronic devices that offer real-time measurements, biological signal processing, and continuous monitoring while maintaining stable performance are in high demand. The materials used in organic electrochemical transistors (OECTs) demonstrate high transconductance (GM) and excellent biocompatibility, making them suitable for bioelectronics in a biological environment. However, ion migration in OECTs induces a delayed response time and low cut-off frequency, and the adverse biological environment causes OECT durability problems. Herein, we present OECTs with a faster response time and improved durability, made possible by using a nanofiber mat channel of a conventional OECT structure. Poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS)/polyacrylamide (PAAm) nanofiber mat channel OECTs are fabricated and subjected to various durability tests for the first time based on continuous measurements and mechanical stability assessments. The results indicate that the nanofiber mat channel OECTs have a faster response time and longer life spans compared to those of film channel OECTs. The improvements can be attributed to the increased surface area and fibrous structure of the nanofiber mat channel. Furthermore, the hydrogel helps to maintain the structure of the nanofiber, facilitates material exchange, and eliminates the need for a crosslinker.

Advanced materials for implantable neuroelectronics.

Materials innovation has arguably played one of the most important roles in the development of implantable neuroelectronics. Such technologies explore biocompatible working systems for reading, triggering, and manipulating neural signals for neuroscience research and provide the additional potential to develop devices for medical diagnostics and/or treatment. The past decade has witnessed a golden era in neuroelectronic materials research. For example, R&D on soft material-based devices have exploded and taken center stage for many applications, including both central and peripheral nerve interfaces. Recent developments have also witnessed the emergence of biodegradable and multifunctional devices. In this article, we aim to overview recent advances in implantable neuroelectronics with an emphasis on chronic biocompatibility, biodegradability, and multifunctionality. In addition to highlighting fundamental materials innovations, we also discuss important challenges and future opportunities.

Electroceuticals for Regeneration of Long Nerve Gap Using Biodegradable Conductive Conduits and Implantable Wireless Stimulator.

Regeneration of over 10 mm long peripheral nerve defects remains a challenge due to the failure of regeneration by prolonged axotomy and denervation occurring in long-term recovery. Recent studies reveal that conductive conduits and electrical stimulation accelerate the regeneration of long nerve defects. In this study, an electroceutical platform combining a fully biodegradable conductive nerve conduit and a wireless electrical stimulator is proposed to maximize the therapeutic effect on nerve regeneration. Fully biodegradable nerve conduit fabricated using molybdenum (Mo) microparticles and polycaprolactone (PCL) can eliminate the unwanted effects of non-degradable implants, which occupy nerve paths and need to be removed through surgery increasing the risk of complications. The electrical and mechanical properties of Mo/PCL conduits are optimized by controlling the amounts of Mo and tetraglycol lubricant. The dissolution behavior and electrical conductivity of biodegradable nerve conduits in the biomimetic solutions are also evaluated. In in vivo experiments, the integrated strategy of a conductive Mo/PCL conduit with controlled therapeutic electrical stimulation shows accelerated axon regeneration for long sciatic nerve defects in rats compared to the use of the Mo/PCL conduit without stimulation and has a significant therapeutic effect based on the results obtained from the functional recovery test.

Three-Dimensionally Printed Expandable Structural Electronics Via Multi-Material Printing Room-Temperature-Vulcanizing (RTV) Silicone/Silver Flake Composite and RTV.

Three-dimensional (3D) printing has various applications in many fields, such as soft electronics, robotic systems, biomedical implants, and the recycling of thermoplastic composite materials. Three-dimensional printing, which was only previously available for prototyping, is currently evolving into a technology that can be utilized by integrating various materials into customized structures in a single step. Owing to the aforementioned advantages, multi-functional 3D objects or multi-material-designed 3D patterns can be fabricated. In this study, we designed and fabricated 3D-printed expandable structural electronics in a substrateless auxetic pattern that can be adapted to multi-dimensional deformation. The printability and electrical conductivity of a stretchable conductor (Ag-RTV composite) were optimized by incorporating a lubricant. The Ag-RTV and RTV were printed in the form of conducting voxels and frame voxels through multi-nozzle printing and were arranged in a negative Poisson's ratio pattern with a missing rib structure, to realize an expandable passive component. In addition, the expandable structural electronics were embedded in a soft actuator via one-step printing, confirming the possibility of fabricating stable interconnections in expanding deformation via a missing rib pattern.

Highly Elastic and Conductive Metallic Interconnect with Crystalline-Amorphous Nanolaminate.

Nanolaminate with alternating layers of nanocrystalline Cu and amorphous CuZrTi is suggested as highly stretchable and conductive interconnect material in stretchable devices. 50 nm nanocrystalline Cu and 20 nm amorphous CuZrTi are the optimum thicknesses of the constituent layers, which result in an elastic deformation limit of 3.33% similar to that of the monolithic amorphous CuZrTi film and an electrical conductivity of 11.83 S/µm corresponding to 70% of that of the monolithic nanocrystalline Cu film. The enhanced elastic deformability and conductivity of the nanolaminates enable the maintenance of the interconnect performance for cyclic stretching with a tensile strain of 114% in the form of a free-standing serpentine structure and a tensile strain of 30% in the form of an ordinary circular coil on an elastomer substrate.

Recent advances in wearable iontronic sensors for healthcare applications.

Iontronic sensors have garnered significant attention as wearable sensors due to their exceptional mechanical performance and the ability to maintain electrical performance under various mechanical stimuli. Iontronic sensors can respond to stimuli like mechanical stimuli, humidity, and temperature, which has led to exploration of their potential as versatile sensors. Here, a comprehensive review of the recent researches and developments on several types of iontronic sensors (e.g., pressure, strain, humidity, temperature, and multi-modal sensors), in terms of their sensing principles, constituent materials, and their healthcare-related applications is provided. The strategies for improving the sensing performance and environmental stability of iontronic sensors through various innovative ionic materials and structural designs are reviewed. This review also provides the healthcare applications of iontronic sensors that have gained increased feasibility and broader applicability due to the improved sensing performance. Lastly, outlook section discusses the current challenges and the future direction in terms of the applicability of the iontronic sensors to the healthcare.

A Personalized Electronic Tattoo for Healthcare Realized by On-the-Spot Assembly of an Intrinsically Conductive and Durable Liquid-Metal Composite.

Conventional electronic (e-) skins are a class of thin-film electronics mainly fabricated in laboratories or factories, which is incapable of rapid and simple customization for personalized healthcare. Here a new class of e-tattoos is introduced that can be directly implemented on the skin by facile one-step coating with various designs at multi-scale depending on the purpose of the user without a substrate. An e-tattoo is realized by attaching Pt-decorated carbon nanotubes on gallium-based liquid-metal particles (CMP) to impose intrinsic electrical conductivity and mechanical durability. Tuning the CMP suspension to have low-zeta potential, excellent wettability, and high-vapor pressure enables conformal and intimate assembly of particles directly on the skin in 10 s. Low-cost, ease of preparation, on-skin compatibility, and multifunctionality of CMP make it highly suitable for e-tattoos. Demonstrations of electrical muscle stimulators, photothermal patches, motion artifact-free electrophysiological sensors, and electrochemical biosensors validate the simplicity, versatility, and reliability of the e-tattoo-based approach in biomedical engineering.

Development of Organic/Inorganic Hybrid Materials for Fully Degradable Reactive Oxygen Species-Releasing Stents for Antirestenosis.

Despite innovative advances in stent technology, restenosis remains a crucial issue for the clinical implantation of stents. Reactive oxygen species (ROS) are known to potentially accelerate re-endothelialization and lower the risk of restenosis by selectively controlling endothelial cells and smooth muscle cells. Recently, several studies have been conducted to develop biodegradable polymeric stents. As biodegradable polymers are not electrically conductive, double metallic layers are required to constitute a galvanic couple for ROS generation. Here, we report a new biodegradable hybrid material composed of a biodegradable polymer substrate and double anodic/cathodic metallic layers for enhancing re-endothelialization and suppressing restenosis. Pure Zn and Mg films (3 µm thick) were deposited onto poly-l-lactic acid (PLLA) substrates by DC magnetron sputtering, and a long-term immersion test using biodegradable hybrid materials was performed in phosphate-buffered solution (PBS) for 2 weeks. The concentrations of superoxide anions and hydrogen peroxide generated by the corrosion of biodegradable metallic films were monitored every 1 or 2 days. Both superoxide anions and hydrogen peroxide were seamlessly generated even after the complete consumption of the anodic Mg layer. It was confirmed that the superoxide anions and hydrogen peroxide were formed not only by the galvanic corrosion between the anode and cathode layers but also by the corrosion of a single Mg or Zn layer. The corrosion products of the Mg and Zn films in PBS were phosphate, oxide, or chloride of the biodegradable metals. Thus, it is concluded that ROS generation by the corrosion of PLLA-based hybrid materials can be sustained until the exhaustion of the cathode metal layer.

Principles for Controlling the Shape Recovery and Degradation Behavior of Biodegradable Shape-Memory Polymers in Biomedical Applications.

Polymers with the shape memory effect possess tremendous potential for application in diverse fields, including aerospace, textiles, robotics, and biomedicine, because of their mechanical properties (softness and flexibility) and chemical tunability. Biodegradable shape memory polymers (BSMPs) have unique benefits of long-term biocompatibility and formation of zero-waste byproducts as the final degradable products are resorbed or absorbed via metabolism or enzyme digestion processes. In addition to their application toward the prevention of biofilm formation or internal tissue damage caused by permanent implant materials and the subsequent need for secondary surgery, which causes secondary infections and complications, BSMPs have been highlighted for minimally invasive medical applications. The properties of BSMPs, including high tunability, thermomechanical properties, shape memory performance, and degradation rate, can be achieved by controlling the combination and content of the comonomer and crystallinity. In addition, the biodegradable chemistry and kinetics of BSMPs, which can be controlled by combining several biodegradable polymers with different hydrolysis chemistry products, such as anhydrides, esters, and carbonates, strongly affect the hydrolytic activity and erosion property. A wide range of applications including self-expending stents, wound closure, drug release systems, and tissue repair, suggests that the BSMPs can be applied as actuators on the basis of their shape recovery and degradation ability.

Fully implantable and bioresorbable cardiac pacemakers without leads or batteries.

Temporary cardiac pacemakers used in periods of need during surgical recovery involve percutaneous leads and externalized hardware that carry risks of infection, constrain patient mobility and may damage the heart during lead removal. Here we report a leadless, battery-free, fully implantable cardiac pacemaker for postoperative control of cardiac rate and rhythm that undergoes complete dissolution and clearance by natural biological processes after a defined operating timeframe. We show that these devices provide effective pacing of hearts of various sizes in mouse, rat, rabbit, canine and human cardiac models, with tailored geometries and operation timescales, powered by wireless energy transfer. This approach overcomes key disadvantages of traditional temporary pacing devices and may serve as the basis for the next generation of postoperative temporary pacing technology.

Biodegradable Metallic Glass for Stretchable Transient Electronics.

Biodegradable electronics are disposable green devices whose constituents decompose into harmless byproducts, leaving no residual waste and minimally invasive medical implants requiring no removal surgery. Stretchable and flexible form factors are essential in biointegrated electronic applications for conformal integration with soft and expandable skins, tissues, and organs. Here a fully biodegradable MgZnCa metallic glass (MG) film is proposed for intrinsically stretchable electrodes with a high yield limit exploiting the advantages of amorphous phases with no crystalline defects. The irregular dissolution behavior of this amorphous alloy regarding electrical conductivity and morphology is investigated in aqueous solutions with different ion species. The MgZnCa MG nanofilm shows high elastic strain (≈2.6% in the nano-tensile test) and offers enhanced stretchability (≈115% when combined with serpentine geometry). The fatigue resistance in repeatable stretching also improves owing to the wide range of the elastic strain limit. Electronic components including the capacitor, inductor, diode, and transistor using the MgZnCa MG electrode support its integrability to transient electronic devices. The biodegradable triboelectric nanogenerator of MgZnCa MG operates stably over 50 000 cycles and its fatigue resistant applications in mechanical energy harvesting are verified. In vitro cell toxicity and in vivo inflammation tests demonstrate the biocompatibility in biointegrated use.

Wirelessly controlled, bioresorbable drug delivery device with active valves that exploit electrochemically triggered crevice corrosion.

Implantable drug release platforms that offer wirelessly programmable control over pharmacokinetics have potential in advanced treatment protocols for hormone imbalances, malignant cancers, diabetic conditions, and others. We present a system with this type of functionality in which the constituent materials undergo complete bioresorption to eliminate device load from the patient after completing the final stage of the release process. Here, bioresorbable polyanhydride reservoirs store drugs in defined reservoirs without leakage until wirelessly triggered valve structures open to allow release. These valves operate through an electrochemical mechanism of geometrically accelerated corrosion induced by passage of electrical current from a wireless, bioresorbable power-harvesting unit. Evaluations in cell cultures demonstrate the efficacy of this technology for the treatment of cancerous tissues by release of the drug doxorubicin. Complete in vivo studies of platforms with multiple, independently controlled release events in live-animal models illustrate capabilities for control of blood glucose levels by timed delivery of insulin.

Bioresorbable pressure sensors protected with thermally grown silicon dioxide for the monitoring of chronic diseases and healing processes.

Pressures in the intracranial, intraocular and intravascular spaces are clinically useful for the diagnosis and management of traumatic brain injury, glaucoma and hypertension, respectively. Conventional devices for measuring these pressures require surgical extraction after a relevant operational time frame. Bioresorbable sensors, by contrast, eliminate this requirement, thereby minimizing the risk of infection, decreasing the costs of care and reducing distress and pain for the patient. However, the operational lifetimes of bioresorbable pressure sensors available at present fall short of many clinical needs. Here, we present materials, device structures and fabrication procedures for bioresorbable pressure sensors with lifetimes exceeding those of previous reports by at least tenfold. We demonstrate measurement accuracies that compare favourably to those of the most sophisticated clinical standards for non-resorbable devices by monitoring intracranial pressures in rats for 25 days. Assessments of the biodistribution of the constituent materials, complete blood counts, blood chemistry and magnetic resonance imaging compatibility confirm the biodegradability and clinical utility of the device. Our findings establish routes for the design and fabrication of bioresorbable pressure monitors that meet requirements for clinical use.

Relation between blood pressure and pulse wave velocity for human arteries.

Continuous monitoring of blood pressure, an essential measure of health status, typically requires complex, costly, and invasive techniques that can expose patients to risks of complications. Continuous, cuffless, and noninvasive blood pressure monitoring methods that correlate measured pulse wave velocity (PWV) to the blood pressure via the Moens-Korteweg (MK) and Hughes Equations, offer promising alternatives. The MK Equation, however, involves two assumptions that do not hold for human arteries, and the Hughes Equation is empirical, without any theoretical basis. The results presented here establish a relation between the blood pressure P and PWV that does not rely on the Hughes Equation nor on the assumptions used in the MK Equation. This relation degenerates to the MK Equation under extremely low blood pressures, and it accurately captures the results of in vitro experiments using artificial blood vessels at comparatively high pressures. For human arteries, which are well characterized by the Fung hyperelastic model, a simple formula between P and PWV is established within the range of human blood pressures. This formula is validated by literature data as well as by experiments on human subjects, with applicability in the determination of blood pressure from PWV in continuous, cuffless, and noninvasive blood pressure monitoring systems.

Wireless bioresorbable electronic system enables sustained nonpharmacological neuroregenerative therapy.

Peripheral nerve injuries represent a significant problem in public health, constituting 2-5% of all trauma cases1. For severe nerve injuries, even advanced forms of clinical intervention often lead to incomplete and unsatisfactory motor and/or sensory function2. Numerous studies report the potential of pharmacological approaches (for example, growth factors, immunosuppressants) to accelerate and enhance nerve regeneration in rodent models3-10. Unfortunately, few have had a positive impact in clinical practice. Direct intraoperative electrical stimulation of injured nerve tissue proximal to the site of repair has been demonstrated to enhance and accelerate functional recovery11,12, suggesting a novel nonpharmacological, bioelectric form of therapy that could complement existing surgical approaches. A significant limitation of this technique is that existing protocols are constrained to intraoperative use and limited therapeutic benefits13. Herein we introduce (i) a platform for wireless, programmable electrical peripheral nerve stimulation, built with a collection of circuit elements and substrates that are entirely bioresorbable and biocompatible, and (ii) the first reported demonstration of enhanced neuroregeneration and functional recovery in rodent models as a result of multiple episodes of electrical stimulation of injured nervous tissue.

Flexible Transient Optical Waveguides and Surface-Wave Biosensors Constructed from Monocrystalline Silicon.

Optical technologies offer important capabilities in both biological research and clinical care. Recent interest is in implantable devices that provide intimate optical coupling to biological tissues for a finite time period and then undergo full bioresorption into benign products, thereby serving as temporary implants for diagnosis and/or therapy. The results presented here establish a silicon-based, bioresorbable photonic platform that relies on thin filaments of monocrystalline silicon encapsulated by polymers as flexible, transient optical waveguides for accurate light delivery and sensing at targeted sites in biological systems. Comprehensive studies of the mechanical and optical properties associated with bending and unfurling the waveguides from wafer-scale sources of materials establish general guidelines in fabrication and design. Monitoring biochemical species such as glucose and tracking physiological parameters such as oxygen saturation using near-infrared spectroscopic methods demonstrate modes of utility in biomedicine. These concepts provide versatile capabilities in biomedical diagnosis, therapy, deep-tissue imaging, and surgery, and suggest a broad range of opportunities for silicon photonics in bioresorbable technologies.

Advanced Materials and Devices for Bioresorbable Electronics.

Recent advances in materials chemistry establish the foundations for unusual classes of electronic systems, characterized by their ability to fully or partially dissolve, disintegrate, or otherwise physically or chemically decompose in a controlled fashion after some defined period of stable operation. Such types of "transient" technologies may enable consumer gadgets that minimize waste streams associated with disposal, implantable sensors that disappear harmlessly in the body, and hardware-secure platforms that prevent unwanted recovery of sensitive data. This second area of opportunity, sometimes referred to as bioresorbable electronics, is of particular interest due to its ability to provide diagnostic or therapeutic function in a manner that can enhance or monitor transient biological processes, such as wound healing, while bypassing risks associated with extended device load on the body or with secondary surgical procedures for removal. Early chemistry research established sets of bioresorbable materials for substrates, encapsulation layers, and dielectrics, along with several options in organic and bio-organic semiconductors. The subsequent realization that nanoscale forms of device-grade monocrystalline silicon, such as silicon nanomembranes (m-Si NMs, or Si NMs) undergo hydrolysis in biofluids to yield biocompatible byproducts over biologically relevant time scales advanced the field by providing immediate routes to high performance operation and versatile, sophisticated levels of function. When combined with bioresorbable conductors, dielectrics, substrates, and encapsulation layers, Si NMs provide the basis for a broad, general class of bioresorbable electronics. Other properties of Si, such as its piezoresistivity and photovoltaic properties, allow other types of bioresorbable devices such as solar cells, strain gauges, pH sensors, and photodetectors. The most advanced bioresorbable devices now exist as complete systems with successful demonstrations of clinically relevant modes of operation in animal models. This Account highlights the foundational materials concepts for this area of technology, starting with the dissolution chemistry and reaction kinetics associated with hydrolysis of Si NMs as a function of temperature, pH, and ion and protein concentration. A following discussion focuses on key supporting materials, including a range of dielectrics, metals, and substrates. As comparatively low performance alternatives to Si NMs, bioresorbable organic semiconductors are also presented, where interest derives from their intrinsic flexibility, low-temperature processability, and ease of chemical modification. Representative examples of encapsulation materials and strategies in passive and active control of device lifetime are then discussed, with various device illustrations. A final section outlines bioresorbable electronics for sensing of various biophysical parameters, monitoring electrophysiological activity, and delivering drugs in a programmed manner. Fundamental research in chemistry remains essential to the development of this emerging field, where continued advances will increase the range of possibilities in sensing, actuation, and power harvesting. Materials for encapsulation layers that can delay water-diffusion and dissolution of active electronics in passively or actively triggered modes are particularly important in addressing areas of opportunity in clinical medicine, and in secure systems for envisioned military and industrial uses. The deep scientific content and the broad range of application opportunities suggest that research in transient electronic materials will remain a growing area of interest to the chemistry community.

CVD-grown monolayer MoS2 in bioabsorbable electronics and biosensors.

Transient electronics represents an emerging technology whose defining feature is an ability to dissolve, disintegrate or otherwise physically disappear in a controlled manner. Envisioned applications include resorbable/degradable biomedical implants, hardware-secure memory devices, and zero-impact environmental sensors. 2D materials may have essential roles in these systems due to their unique mechanical, thermal, electrical, and optical properties. Here, we study the bioabsorption of CVD-grown monolayer MoS2, including long-term cytotoxicity and immunological biocompatibility evaluations in biofluids and tissues of live animal models. The results show that MoS2 undergoes hydrolysis slowly in aqueous solutions without adverse biological effects. We also present a class of MoS2-based bioabsorbable and multi-functional sensor for intracranial monitoring of pressure, temperature, strain, and motion in animal models. Such technology offers specific, clinically relevant roles in diagnostic/therapeutic functions during recovery from traumatic brain injury. Our findings support the broader use of 2D materials in transient electronics and qualitatively expand the design options in other areas.