Jamming of Miscible Liquids via Electrostatic Repulsion Between Polystyrene-Modified Gold Nanorods and Toluene.

Structured liquids in miscible fluids, due to ineffective resistance to withstand particle self-diffusion, differ from that in immiscible liquids because of interfacial interactions. Here, a kind of structured liquid, jammed by thiol-terminated polystyrene-modified gold nanorods (GNRs) within tetrahydrofuran and toluene (TOL), is developed by introducing electrostatic repulsion to counterbalance the self-diffusion of GNRs. First-principle calculations reveal charge transfer between the GNRs and TOL, resulting in the electrostatic repulsion. The structured liquids can be regarded as mimic "loading vehicles" to controllably carry and transport matter under electric or magnetic fields, where release rate can be adjusted by changing the concentration of the soluble matter for slow release and using the photothermal effect of the assembled GNRs for fast release. This work has developed a new assembly mechanism to form structured liquids, allowing the construction of a flexible and robust droplet platform with possible applications in microreactors, biomimetic permeable membranes, and functional liquid robots.

Wide-Humidity Range Applicable, Anti-Freezing, and Healable Zwitterionic Hydrogels for Ion-Leakage-Free Iontronic Sensors.

Hydrogels have entered the spotlight for applications in soft electronics. It is essential and challenging to obtain hydrogels that can function properly under varying environmental circumstances, that is, 30-90% relative humidity (RH) and -20 to 40 °C due to their intrinsic nature to lose and absorb water upon variations in humidity and temperature. In this work, a green solvent, solketal, is introduced into poly 3-dimethyl-2-(2-methylprop-2-enoyloxy)ethyl azaniumyl propane-1-sulfonate (poly(DMAPS)) zwitterionic hydrogels. Compared to glycerol, solketal endows hydrogels with greater possibility for further modification as well as improved water content and mechanical performance consistency over 30-90% RH. Encouragingly, the optimized hydrogel demonstrates its unique merits as a dielectric layer in iontronic sensors, featuring non-leaky ions, high sensitivity (1100 kPa-1 ), wide humidity, and temperature range applicability. A wide-humidity range healable and stretchable electrode is attained by combining the hydrogel substrate with Ag paste. A full-device healable and highly-sensitive sensor is developed. This study is a pioneering work that tackles the broad humidity range applicability issue of hydrogels, and demonstrates the ion-leakage-free ionic skins with zwitterionic dielectrics. The outcomes of the study will considerably promote advancements in the fields of hydrogel electronics and iontronic sensors.

Bioinspired Multimodal Multipose Hybrid Fingers for Wide-Range Force, Compliant, and Stable Grasping.

The increasing demand for grasping diverse objects in unstructured environments poses severe challenges to the existing soft/rigid robotic fingers due to the issues in balancing force, compliance, and stability, and hence has given birth to several hybrid designs. These hybrid designs utilize the advantages of rigid and soft structures and show better performance, but they are still suffering from narrow output force range, limited compliance, and rarely reported stability. Owing to its rigid-soft coupling structure with flexible switched multiple poses, human finger, as an excellent hybrid design, shows wide-range output force, excellent compliance, and stability. Inspired by human finger, we propose a hybrid finger with multiple modes and poses, coupled by a soft actuator (SA) and a rigid actuator (RA) in parallel. The multiple actuation modes formed by a pneumatic-based rigid-soft collaborative strategy can selectively enable the RA's high force and SA's softness, whereas the multiple poses derived from the specially designed underactuated RA skeleton can be flexibly switched with tasks, thus achieving high compliance. Such hybrid fingers also proved to be highly stable under external stimuli or gravity. Furthermore, we modularize and configure these fingers into a series of grippers with excellent grasping performance, for example, wide graspable object range (diverse from 0.1 g potato chips to 27 kg dumbbells for a 420 g two-finger gripper), high compliance (tolerate objects with 94% gripper span size and 4 cm offset), and high stability. Our study highlights the potential of fusing rigid-soft technologies for robot development, and potentially impacts future bionics and high-performance robot development.

Ultrathin Hydrogel Films toward Breathable Skin-Integrated Electronics.

On-skin electronics that offer revolutionary capabilities in personalized diagnosis, therapeutics, and human-machine interfaces require seamless integration between the skin and electronics. A common question remains whether an ideal interface can be introduced to directly bridge thin-film electronics with the soft skin, allowing the skin to breathe freely and the skin-integrated electronics to function stably. Here, an ever-thinnest hydrogel is reported that is compliant to the glyphic lines and subtle minutiae on the skin without forming air gaps, produced by a facile cold-lamination method. The hydrogels exhibit high water-vapor permeability, allowing nearly unimpeded transepidermal water loss and free breathing of the skin underneath. Hydrogel-interfaced flexible (opto)electronics without causing skin irritation or accelerated device performance deterioration are demonstrated. The long-term applicability is recorded for over one week. With combined features of extreme mechanical compliance, high permeability, and biocompatibility, the ultrathin hydrogel interface promotes the general applicability of skin-integrated electronics.

Multimaterial Three-Dimensional Printing of Ultraviolet-Curable Ionic Conductive Elastomers with Diverse Polymers for Multifunctional Flexible Electronics.

Ionic conductive elastomers (ICEs) are emerging stretchable and ionic conductive materials that are solvent-free and thus demonstrate excellent thermal stability. Three-dimensional (3D) printing that creates complex 3D structures in free forms is considered as an ideal approach to manufacture sophisticated ICE-based devices. However, the current technologies constrain 3D printed ICE structures in a single material, which greatly limits functionality and performance of ICE-based devices and machines. Here, we report a digital light processing (DLP)-based multimaterial 3D printing capability to seemly integrate ultraviolet-curable ICE (UV-ICE) with nonconductive materials to create ionic flexible electronic devices in 3D forms with enhanced performance. This unique capability allows us to readily manufacture various 3D flexible electronic devices. To demonstrate this, we printed UV-ICE circuits into polymer substrates with different mechanical properties to create resistive strain and force sensors; we printed flexible capacitive sensors with high sensitivity (2 kPa-1) and a wide range of measured pressures (from 5 Pa to 550 kPa) by creating a complex microstructure in the dielectric layer; we even realized ionic conductor-activated four-dimensional (4D) printing by printing a UV-ICE circuit into a shape memory polymer substrate. The proposed approach paves a new efficient way to realize multifunctional flexible devices and machines by bonding ICEs with other polymers in 3D forms.

Tailoring Poly(Styrene-co-maleic anhydride) Networks for All-Polymer Dielectrics Exhibiting Ultrahigh Energy Density and Charge-Discharge Efficiency at Elevated Temperatures.

Polymer film capacitors have been widely used in electronics and electrical power systems due to their advantages of high power densities, fast charge-discharge speed, and great stability. However, the exponential increase of electrical conduction with temperature and applied electric field substantially degrades the capacitive performance of dielectric polymers at elevated temperatures. Here, the first example of controlling the energy level of charge traps in all-organic crosslinked polymers by tailoring molecular structures that significantly inhibit high-field high-temperature conduction loss, which largely differs from current approaches based on the introduction of inorganic fillers, is reported. The polymer network with optimized crosslinking structures exhibits an ultrahigh discharged energy density of 7.02 J cm-3 with charge/discharge efficiencies of >90% at 150 °C, far outperforming current dielectric polymers and composites. The charge-trapping effects in different crosslinked structures, as the origins of the marked improvements in the high-temperature capacitive performance, are comprehensively investigated experimentally and confirmed computationally. Moreover, excellent cyclability and self-healing features are demonstrated in the polymer film capacitors. This work offers a promising pathway of molecular structure design to scalable high-energy-density polymer dielectrics capable of operating under harsh environments.

Adhesion-Shielding based synthesis of interfacially active magnetic Janus nanoparticles.

HYPOTHESIS: A unique adhesion-shielding (AS)-based method could be used to manufacture magnetic Janus nanoparticles (IM-JNPs) of promising interfacial activities, asymmetric surface wettability, and great performance on deoiling from oily wastewater under the external magnetic field. EXPERIMENTS: The IM-JNPs were characterized using scanning electron microscope (SEM), X-ray diffraction (XRD), thermogravimetric analysis (TGA), and Fourier-transform infrared spectroscopy (FTIR). The interfacial properties of IM-JNPs were investigated by the measurements of interfacial pressure-area isotherms (π-A), oil-water interfacial tension, and the related crumpling ratio. The Langmuir-Blodgett (L-B) technique was used to determine the asymmetric surface wettability of the IM-JNPs. The performance and recyclability of IM-JNPs for treating oily wastewater were also investigated. FINDINGS: Using the proposed AS-based method, 17.9 g IM-JNPs were synthesized at a time and exhibited excellent interfacial properties, as indicated by decreasing oil-water interfacial tension from 38 to 27 mN/m. The crumpling behavior of the oil droplet further demonstrated the irreversible deposition of IM-JNPs at the oil droplet surfaces. The L-B technique and water contact angle measurement confirmed the asymmetric surface wettability of the IM-JNPs. The IM-JNPs were applied to successful removal of > 90% emulsified oil droplets from the household-produced oily wastewater under the external magnetic field while realizing facile recyclability and regeneration.

Leaf-Inspired Flexible Thermoelectric Generators with High Temperature Difference Utilization Ratio and Output Power in Ambient Air.

The inherently small temperature difference in air environment restricts the applications of thermoelectric generation in the field of Internet of Things and wearable electronics. Here, a leaf-inspired flexible thermoelectric generator (leaf-TEG) that makes maximum use of temperature difference by vertically aligning poly(3,4-ethylenedioxythiophene) polystyrene sulfonate and constantan thin films is demonstrated. Analytical formulae of the performance scales, i.e., temperature difference utilization ratio (φth) and maximum output power (Pmax), are derived to optimize the leaf-TEG dimensions. In an air duct (substrate: 36 °C, air: 6 °C, air flowing: 1 m s-1), the 10-leaf-TEG shows a φth of 73% and Pmax of 0.38 µW per leaf. A proof-of-concept wearable 100-leaf-TEG (60 cm2) generates 11 µW on an arm at room temperature. Furthermore, the leaf-TEG is flexible and durable that is confirmed by bending and brushing over 1000 times. The proposed leaf-TEG is very appropriate for air convection scenarios with limited temperature differences.

High-Performance Liquid Alloy Patterning of Epidermal Strain Sensors for Local Fine Skin Movement Monitoring.

Nowadays, stretchable/epidermal electronics based on liquid alloys has attracted more and more attention, and various processing techniques have subsequently been developed to demonstrate diverse applications never seen before. However, to fully exploit its potential advantages, epidermal electronics is still searching for a technique meeting all demands on resolution, pattern complexity, and operational flexibility. In this study, we propose a technique that allows for complex and high-density patterns on thin stretchable substrates by combining ultraviolet laser patterning of a modified water-soluble mask, atomized spray deposition of liquid alloys on a flexible temporary substrate, lift-off by water dissolving, and finally, component integration and encapsulation. With this new technique, it was possible to make epidermal precision strain sensors with liquid alloy patterns of high density, which were capable of monitoring fine local skin movements such as the detailed process of wrinkle formation as well as the overall motion of the body part. In addition, this process is highly efficient and well controllable, with high potential for possible industrial automation and massive production.

Tunnel Encapsulation Technology for Durability Improvement in Stretchable Electronics Fabrication.

Great diversity of process technologies and materials have been developed around stretchable electronics. A subset of them, which are made up of zigzag metal foil and soft silicon polymers, show advantages of being easy to manufacture and low cost. However, most of the circuits lack durability due to stress concentration of interconnects entirely embedded in elastic polymer silicone such as polydimethylsiloxane (PDMS). In our demonstration, tunnel encapsulation technology was introduced to relieve stress of these conductors when they were stretched to deform in and out of plane. It was realized by dissolving the medium of Polyvinyl Alcohol (PVA), previous cured together with circuits in polymer, to form the micro-tunnel which not only guarantee the stretchability of interconnect, but also help to improve the durability. With the protection of tunnel, the serpentine could stably maintain the designed shape and electrical performance after 50% strain cycling over 20,000 times. Finally, different materials for encapsulation were employed to provide promising options for applications in portable biomedical devices which demand duplicate distortion.

Realization of near-perfect absorption in the whole reststrahlen band of SiC.

Materials used for outdoor radiative cooling technologies need not only be transparent in the solar spectral region, but also need to have a broadband perfect absorption in the infrared atmospheric transparency window (infrared-ATW). Silicon carbide (SiC) has been thought to be a potential candidate for such materials. However, due to the near-perfect reflection of electromagnetic waves in the whole reststrahlen band (RB) of SiC, which is within the infrared-ATW, perfect absorption in the whole RB remains a challenge. Here by constructing a cone-pillar double-structure surface on SiC, a near-perfect absorption (>97%) of normally incident electromagnetic waves in the whole RB has been realized experimentally. Simulation results reveal that the dominant reason for the near-perfect absorption is the efficient coupling of incident electromagnetic waves into the bulk evanescent waves in the free-space wavelength range (10.33 µm, 10.55 µm) and the efficient coupling of incident electromagnetic waves into the surface phonon polaritons in the free-space wavelength range (10.55 µm, 12.6 µm). Our findings open up an avenue to enhance the absorption performance of SiC in infrared-ATW, and may lead to many new applications.

On-Demand Multi-Resolution Liquid Alloy Printing Based on Viscoelastic Flow Squeezing.

Recently, high-resolution patterning techniques of stretchable electronics advanced extensively. An important trend is to fabricate complex circuits with varied sizes in a small area, which is a technical challenge to current conductive ink printing technologies. Here, we introduce a new strategy for multi-resolution liquid alloy printing, which can tune the resolution of printed liquid alloy trace in real time with the squeezing effect of compound viscoelastic flow. A newly developed coaxial nozzle with the inner nozzle extension (CNINE) is used to wrap and squeeze liquid alloy steadily and effectively. By controlling the working parameters and compound flow properties, liquid alloy patterns with different widths are obtained continuously. This work offers a new way to rapidly manufacture complex stretchable electronics patterning in multi-resolution.

Symmetry control of nanorod superlattice driven by a governing force.

Nanoparticle self-assembly promises scalable fabrication of composite materials with unique properties, but symmetry control of assembled structures remains a challenge. By introducing a governing force in the assembly process, we develop a strategy to control assembly symmetry. As a demonstration, we realize the tetragonal superlattice of octagonal gold nanorods, breaking through the only hexagonal symmetry of the superlattice so far. Surprisingly, such sparse tetragonal superstructure exhibits much higher thermostability than its close-packed hexagonal counterpart. Multiscale modeling reveals that the governing force arises from hierarchical molecular and colloidal interactions. This force dominates the interactions involved in the assembly process and determines the superlattice symmetry, leading to the tetragonal superlattice that becomes energetically favorable over its hexagonal counterpart. This strategy might be instructive for designing assembly of various nanoparticles and may open up a new avenue for realizing diverse assembly structures with pre-engineered properties.

Nanostructured YbAgCu4 for potentially cryogenic thermoelectric cooling.

We have studied the thermoelectric properties of nanostructured YbAgCu4 materials. A high power factor of ∼131 µW cm(-1) K(-2) has been obtained at 22 K for nanostructured samples prepared by ball milling the arc melted ingot into nanopowder and hot pressing the nanopowder. The implementation of nanostructuring method decreased the thermal conductivity at 42 K by 30-50% through boundary scattering comparing with the previously reported value of polycrystalline YbAgCu4. A peak dimensionless thermoelectric figure-of-merit, ZT, of 0.11 has been achieved at 42 K, which may find potential applications for cryogenic cooling below 77 K. The nanostructuring approach can be extended to other heavy Fermion materials to achieve high power factor and low thermal conductivity and ultimately higher ZT.

Thermoelectric performance of Ni compensated cerium and neodymium double filled p-type skutterudites.

We have synthesized Ni compensated Ce and Nd double filled p-type skutterudites CexNdxFe3.7Ni0.3Sb12 with x = 0.35, 0.40, 0.45, and 0.5 by a melting-quenching-annealing method. The samples were made by directly hot pressing the hand ground powder at 650 °C for 5 minutes at a pressure of about 80 MPa. Since Ni has two more electrons than Fe, a lower power factor and a stronger bipolar effect in thermal conductivity are expected at higher temperature. In the experiments, we have demonstrated that by suitably tuning the Fe-Ni ratio and filler concentration, we can achieve both a higher power factor (∼35 µW cm(-1) K(-2) at 535 °C) and a lower thermal conductivity (∼2.1 W m(-1) K(-1) at room temperature and ∼2.7 W m(-1) K(-1) at 535 °C) in Ce0.4Nd0.4Fe3.7Ni0.3Sb12. A peak thermoelectric figure-of-merit of ∼1.1 at 475 °C is achieved in Ce0.4Nd0.4Fe3.7Ni0.3Sb12.

Uniform self-forming metallic network as a high-performance transparent conductive electrode.

A transparent, conductive, and flexible electrode is demonstrated. It is based on an inexpensive and easily manufacturable metallic network formed by depositing metals onto a template film. This electrode shows excellent electro-optical properties, with the figure of merit ranging from 300 to 700, and transmittance from 82% (~4.3 Ω sq(-1) ) to 45% (~0.5 Ω sq(-1) ).

One-step fabrication of micro/nanotunnels in metal interlayers.

A micro/nanotunnel is a very useful structure, which has been used as an interconnected pass in various micro/nano systems. Here, a novel micro/nanotunnel fabrication method in a metal interlayer ZnS-SiO2/Sn/ZnS-SiO2 sandwich structure is proposed based on a laser direct writing (LDW) technique. The experimental results show that the arched tunnel is 170 nm in width and 50 nm in height, far beyond the diffraction limit of the LDW system with a 533 nm laser and 0.9 NA objective lens. In only one step, an arbitrary tunnel can be fabricated, exhibiting its simple, designable and practical features, and providing a new route for micro/nanotunnel fabrication.

Controllable two-stage droplet evaporation method and its nanoparticle self-assembly mechanism.

Bottom-up self-assembly is able to constitute a variety of structures and has been thought to be a promising way for advanced nanofabrication. Droplet evaporation, as the simplest method, has been used in various self-assemblies. However, the assembled area is not large enough and the order is still not well controlled. Here we show a facile and controllable two-stage droplet evaporation method by adjusting the humidity and temperature of the evaporating droplet. Taking the highly monodispersed gold nanorods (GNRs) as an example, large-area, self-assembly monolayer arrays are reproducibly achieved. To understand the self-assembly mechanism, we adopted simplified models to analyze the interactions between the nanorods. The results show that a metastable state of secondary-energy-minimum exists, especially in the latter stage of the assembly process, leading to the ordered arrays. A large electrostatic barrier between the assembled arrays prevents the formation of the multilayer structures and thereby leads to the preferential monolayers. Moreover, we predict possibilities of different types of assemblies of the nanorods, and a schematic phase diagram is finally given. The results here may offer a way toward high-quality self-assembled nanoparticles superlattices for use in enhanced spectroscopy, sensors, or nanodevices.

Modified chemical vapor deposition synthesis of ultralong V2O5 nanobelt and its electronic properties.

The fascinating properties and wide applications of the V2O5 nanostructures have attracted significant attention over the past decades. In this paper, ultralong (centimeter-scale) single-crystal V2O5 nanobelts are successfully fabricated by modified chemical vapor deposition. The wide of the V2O5 nanobelts are 20-500 nm. The aspect ratio exceeds 10(5). The structure and crystal orientation of the nanobelts are investigated. X-ray diffractometer (XRD) patterns and Raman spectrum show the substrate temperature affecting the size and morphology of the V2O5 nanobelts. And the growth mechanism and electronic properties of the ultralong V2O5 nanobelt are studied in detail. The activation energy 0.12 eV is calculated. The fastest growth orientation along the [010] direction has been observed. Our work demonstrates that the single-crystal V2O5 nanobelt has potential applications in field-emitters, lithium-ion batteries, photodetectors, interconnect, and optoelectronic devices, etc.

A high quality BiOCl film with petal-like hierarchical structures and its visible-light photocatalytic property.

BiOCl film with petal-like hierarchical structures is obtained by dipping bismuth film into the mixed solution of H2O2 and HCl. To obtain a high quality BiOCI film, a connecting layer of Chromium is deposited between the substrate and Bismuth film. The product is easy-synthesized, high productive, reusable and environment-friendly. The structural analysis indicates that the BiOCI film is composed by petals with smooth surfaces, and the nanopetals grow along the (101) directions. Raman spectroscopy shows that the film has a good stress-resist feature. The PL spectrum shows that the defect energy levels of BiOCI nanostructure contribute to the excellent photoactivity of degradation the rhodamine B (RhB) under visible-light irradiation (A > 420 nm). This photocatalyst can keep stable photoactivity after it has been reused for 6 rounds. All those properties ensure the photocatalyst a bright future in the application of the pollution treatment.