Superstrong Ionogel Enabled by Coacervation-Induced Nanofibril Assembly for Sustainable Moisture Energy Harvesting.

Ionogels have grabbed significant interest in various applications, from sensors and actuators to wearable electronics and energy storage devices. However, current ionogels suffer from low strength and poor ionic conductivity, limiting their performance in practical applications. Here, inspired by the mechanical reinforcement of natural biomacromolecules through noncovalent aggregates, a strategy is proposed to construct nanofibril-based ionogels through complex coacervation-induced assembly. Cellulose nanofibrils (CNFs) can bundle together with poly(ionic liquid) (PIL) to form a superstrong nanofibrous network, in which the ionic liquid (IL) can be retained to form ionogels with high liquid inclusion and ionic conductivity. The strength of the CNF-PIL-IL ionogels can be tuned by the IL content over a wide range of up to 78 MPa. The optical transparency, high strength, and hygroscopicity enabled them to be promising candidates in moist-electricity generation and applications such as energy harvesting windows and wearable power generators. In addition, the ionogels are degradable and the ionogel-based generators can be recycled through dehydration. Our strategy suggests perspectives for the fabrication of high-strength and multifunctional ionogels for sustainable applications.

On-chip droplet analysis and cell spheroid screening by capillary wrapping enabled shape-adaptive ferrofluid transporters.

Non-invasive droplet manipulation with no physical damage to the sample is important for the practical value of manipulation tools in multidisciplinary applications from biochemical analysis and diagnostics to cell engineering. It is a challenge to achieve this for most existing photothermal, electric stimuli, and magnetic field-based technologies. Herein, we present a droplet handling toolbox, the ferrofluid transporter, for non-invasive droplet manipulation in an oil environment. It involves the transport of droplets with high robustness and efficiency owing to low interfacial friction. This capability caters to various scenarios including droplets with varying components and solid cargo. Moreover, we fabricated a droplet array by transporter positioning and achieved droplet gating and sorting for complex manipulation in the droplet array. Benefiting from the ease of scale-up and high biocompatibility, the transporter-based droplet array can serve as a digital microfluidic platform for on-chip droplet-based bioanalysis, cell spheroid culture, and downstream drug screening tests.

Tough soldering for stretchable electronics by small-molecule modulated interfacial assemblies.

The rapid-developing soft robots and wearable devices require flexible conductive materials to maintain electric functions over a large range of deformations. Considerable efforts are made to develop stretchable conductive materials; little attention is paid to the frequent failures of integrated circuits caused by the interface mismatch of soft substrates and rigid silicon-based microelectronics. Here, we present a stretchable solder with good weldability that can strongly bond with electronic components, benefiting from the hierarchical assemblies of liquid metal particles, small-molecule modulators, and non-covalently crosslinked polymer matrix. Our self-solder shows high conductivity (>2×105 S m-1), extreme stretchability (~1000%, and >600% with chip-integrated), and high toughness (~20 MJ m-3). Additionally, the dynamic interactions within our solder's surface and interior enable a range of unique features, including ease of integration, component substitution, and circuit recyclability. With all these features, we demonstrated an application as thermoforming technology for three-dimensional (3D) conformable electronics, showing potential in reducing the complexity of microchip interfacing, as well as scalable fabrication of chip-integrated stretchable circuits and 3D electronics.

Microphase-Separated Elastic and Ultrastretchable Ionogel for Reliable Ionic Skin with Multimodal Sensation.

Bioinspired artificial skins integrated with reliable human-machine interfaces and stretchable electronic systems have attracted considerable attention. However, the current design faces difficulties in simultaneously achieving satisfactory skin-like mechanical compliance and self-powered multimodal sensing. Here, this work reports a microphase-separated bicontinuous ionogel which possesses skin-like mechanical properties and mimics the multimodal sensing ability of biological skin by ion-driven stimuli-electricity conversion. The ionogel exhibits excellent elasticity and ionic conductivity, high toughness, and ultrastretchability, as well as a Young's modulus similar to that of human skin. Leveraging the ion-polymer interactions enabled selective ion transport, the ionogel can output pulsing or continuous electrical signals in response to diverse stimuli such as strain, touch pressure, and temperature sensitively, demonstrating a unique self-powered multimodal sensing. Furthermore, the ionogel-based I-skin can concurrently sense different stimuli and decouple the variations of the stimuli from the voltage signals with the assistance of a machine-learning model. The ease of fabrication, wide tunability, self-powered multimodal sensing, and the excellent environmental tolerance of the ionogels demonstrate a new strategy in the development of next-generation soft smart mechano-transduction devices.

Press-N-Go On-Skin Sensor with High Interfacial Toughness for Continuous Healthcare Monitoring.

On-skin electronic sensors are demanded for healthcare monitoring such as the continuous recording of biopotential and motion signals from patients. However, the mechanical mismatches and poor interface adhesion at the skin/sensor interfaces always cause high interfacial impedance and artifacts, frequent interfacial failure, and unexpected depletion of the device, which significantly limit the performance of the sensors. We here develop an on-skin sensor based on a conductive pressure-sensitive tape, which is assembled from supramolecular dual-cross-linked hydrogel composites. Both covalent and noncovalent cross-links in the hydrogel networks could harvest high flexibility, pressure-sensitive adhesion, and high interfacial toughness altogether, enabling a convenient "Press-N-Go" application of the sensor on human skin without additional pre/post-treatment on the skin or the senor. The high conformability and low resistivity of the tape can sustainably lower the interfacial impedance and thus improve signal quality in various measurement conditions. Our design provides a feasible path to develop interface-toughened on-skin electronics, which is desired in dynamic human-machine interfaces.

Liquid Metal Nanoparticles as a Highly Efficient Photoinitiator to Develop Multifunctional Hydrogel Composites.

Liquid metal (LM) composites are a class of emerging soft multifunctional materials that are promising for a variety of applications, yet the chemistry properties of LM have not been fully understood. Here, we report that LM nanoparticles can directly perform as a photoinitiator for radical polymerization and the in situ development of highly tough and multifunctional LM hydrogel composites. It is revealed that the photocatalytic activity of LM nanoparticles originates from the oxide layer on LM. Significantly, positively charged metal-organic framework (MOF) nanoparticles are used to stabilize LM nanoparticles in aqueous solutions, where the MOF can anchor on the surface of LM nanoparticles by electrostatic interaction while helping to preserve the unshielded oxide layer, therefore realizing the highly efficient photoinitiation and polymerization. The LM nanoparticle-initiated photopolymerization is shown to develop hydrogel composites featuring excellent stretchability, stimuli responsiveness, and sustained photocatalytic activity. The photocatalytic polymerization initiated by LM nanoparticles not only deepens the understanding on the semiconductor properties of the oxide skin on LM but also broadens the application scenarios of multifunctional LM/polymer composites in smart materials, wearable electronics, and soft robotics.

Wetting ridge assisted programmed magnetic actuation of droplets on ferrofluid-infused surface.

Flexible actuation of droplets is crucial for biomedical and industrial applications. Hence, various approaches using optical, electrical, and magnetic forces have been exploited to actuate droplets. For broad applicability, an ideal approach should be programmable and be able to actuate droplets of arbitrary size and composition. Here we present an "additive-free" magnetic actuation method to programmably manipulate droplets of water, organic, and biological fluids of arbitrary composition, as well as solid samples, on a ferrofluid-infused porous surface. We specifically exploit the spontaneously formed ferrofluid wetting ridges to actuate droplets using spatially varying magnetic fields. We demonstrate programmed processing and analysis of biological samples in individual drops as well as the collective actuation of large ensembles of micrometer-sized droplets. Such model respiratory droplets can be accumulated for improved quantitative and sensitive bioanalysis - an otherwise prohibitively difficult task that may be useful in tracking coronavirus.

Ultrastretchable conductive liquid metal composites enabled by adaptive interfacial polarization.

Gallium-based liquid metals (LMs) are emerging candidates for the development of metal/polymer-based flexible circuits in wearable electronics. However, the high surface energies of LMs make them easily depleted from the polymer matrix and therefore substantially suppress the stretchability of the conductive composites. Here, we reveal that a dynamic interplay between the LM and the polyvinylidene fluoride (PVDF) copolymer can help to address these issues. Weak and abundant interfacial polarization interactions between the PVDF copolymer and the oxide layer allow continuous and adaptive configuration of the compartmented LM channels, enabling ultra-stretchability of the composites. The conductive LM-polymer composites can maintain their structural integrity with a high surface conductivity and small resistance changes under large strains from 1000% to 10 000%. Taking advantage of their flexible processability under mild conditions and exceptional performance, our design strategy allows the scalable fabrication of conductive LM-polymer composites for a range of applications in wearable devices and sensors.

Borohydride catalyzed redistribution reaction of hydrosilane and chlorosilane: a potential system for facile preparation of hydrochlorosilanes.

Various borohydrides were found to catalyze the redistribution reaction of hydrosilane and chlorosilane in different solvents to produce hydrochlorosilanes efficiently and facilely. The redistribution reaction was affected by solvent and catalyst. The substrate scope was investigated in HMPA with LiBH4 as catalyst. A possible mechanism was proposed to explain the redistribution process.

Synthesis of structured polysiloxazanes via a Piers-Rubinsztajn reaction.

A series of siloxazanes were successfully prepared by a Piers-Rubinsztajn reaction between methoxydisilazanes and the corresponding hydrosilanes. Polysiloxazanes with narrow dispersion were also synthesized from methoxydisilazanes and Si-H terminated oligosiloxanes. The possible interaction mechanism between tris(pentafluorophenyl)borane and the methoxydisilazane was investigated.