Omniphobic “RF Paper” Produced by Silanization of Paper with Fluoroalkyltrichlorosilanes

The fabrication and properties of “fluoroalkylated paper” (“R^F paper”) by vapor‐phase silanization of paper with fluoroalkyl trichlorosilanes is reported. R^F paper is both hydrophobic and oleophobic: it repels water (θ_app^H2^O>140°), organic liquids with surface tensions as low as 28 mN m^‐1, aqueous solutions containing ionic and non‐ionic surfactants, and complex liquids such as blood (which contains salts, surfactants, and biological material such as cells, proteins, and lipids). The propensity of the paper to resist wetting by liquids with a wide range of surface tensions correlates with the length and degree of fluorination of the organosilane (with a few exceptions in the case of methyl trichlorosilane‐treated paper), and with the roughness of the paper. R^F paper maintains the high permeability to gases and mechanical flexibility of the untreated paper, and can be folded into functional shapes (e.g., microtiter plates and liquid‐filled gas sensors). When impregnated with a perfluorinated oil, R^F paper forms a “slippery” surface (paper slippery liquid‐infused porous surface, or “paper SLIPS“) capable of repelling liquids with surface tensions as low as 15 mN m^‐1. The foldability of the paper SLIPS allows the fabrication of channels and flow switches to guide the transport of liquid droplets.     

Dry‐Type Artificial Muscles Based on Pendent Sulfonated Chitosan and Functionalized Graphene Oxide for Greatly Enhanced Ionic Interactions and Mechanical Stiffness

Biopolymer‐based artificial muscles are promising candidates for biomedical applications and smart electronic textiles due to their multifaceted advantages like natural abundance, eco‐friendliness, cost‐effectiveness, easy chemical modification and high electical reactivity. However, the biopolymer‐based actuators are showing relatively low actuation performance compared with synthetic electroactive polymers because of inadequate mechanical stiffness, low ionic conductivity and ionic exchange capacity (IEC), and poor durability over long‐term activation. This paper reports a high‐performance electro‐active nano‐biopolymer based on pendent sulfonated chitosan (PSC) and functionalized graphene oxide (GO), exhibiting strong electro‐chemo‐mechanical interations with ionic liquid (IL) in open air environment. The proposed GO‐PSC‐IL nano‐biopolymer membrane shows an icnreased tensile strength and ionic exchange capacity of up to 44.8% and 83.1%, respectively, and increased ionic conductivity of over 18 times, resulting in two times larger bending actuation than the pure chitosan actuator under electrical input signals. Eventually, the GO‐PSC‐IL actuators could show robust and high‐performance actuation even at the very low applied voltages that are required in realistic applications.     

Design and Synthesis of “All‐in‐One” Multifunctional FeS2 Nanoparticles for Magnetic Resonance and Near‐Infrared Imaging Guided Photothermal Therapy of Tumors

The ideal theranostic nanoplatform for tumors is a single nanoparticle that has a single semiconductor or metal component and contains all multimodel imaging and therapy abilities. The design and preparation of such a nanoparticle remains a serious challenge. Here, with FeS₂ as a model of a semiconductor, the tuning of vacancy concentrations for obtaining “all‐in‐one” type FeS₂ nanoparticles is reported. FeS₂ nanoparticles with size of ≈30 nm have decreased photoabsorption intensity from the visible to near‐infrared (NIR) region, due to a low S vacancy concentration. By tuning their shape/size and then enhancing the S vacancy concentration, the photoabsorption intensity of FeS₂ nanoparticles with size of ≈350 nm (FeS₂‐350) goes up with the increase of the wavelength from 550 to 950 nm, conferring the high NIR photothermal effect for thermal imaging. Furthermore, this nanoparticle has excellent magnetic properties for T₂‐weighted magnetic resonance imaging (MRI). Subsequently, FeS₂‐350 phosphate buffer saline (PBS) dispersion is injected into the tumor‐bearing mice. Under the irradiation of 915‐nm laser, the tumor can be ablated and the metastasis lesions in liver suffer significant inhibition. Therefore, FeS₂‐350 has great potential to be used as novel “all‐in‐one” multifunctional theranostic nanoagents for MRI and NIR dual‐modal imaging guided NIR‐photothermal ablation therapy (PAT) of tumors.     

Enhanced Variable Stiffness and Variable Stretchability Enabled by Phase‐Changing Particulate Additives

A novel phase‐changing particulate that amplifies a composite's modulus change in response to thermal stimulus is introduced. This particulate additive consists of a low melting point alloy (Field's metal; FM) formed into microparticles using a facile fabrication method, which enables its incorporation into polymer matrices using simple composite manufacturing processes. The effect of the solid–liquid phase change of the FM particles is demonstrated in two host materials: a thermally responsive epoxy and a silicone elastomer. In the epoxy matrix, this thermal response manifests as an amplified change in flexural modulus when heated, which is highly desirable for stiffness‐changing move‐and‐hold applications. In the silicone matrix, the stretchability can be switched depending on the phase of the FM particles. This phenomenon allows the silicone to stretch and hold a strained configuration, and gives rise to mechanically programmable anisotropy through reshaping of the FM inclusions. FM particles present many opportunities where on‐demand tunable modulus is required, and is particularly relevant to soft robotics. Because the melting temperature of FM is near room temperature, triggering the phase change requires low power consumption. The utility of FM particle‐containing composites as variable stiffness and variable stretchability elements for soft robotic applications is demonstrated.     

Elastically and Plastically Foldable Electrothermal Micro‐Origami for Controllable and Rapid Shape Morphing

Integrating origami principles within traditional microfabrication methods can produce shape morphing microscale metamaterials and 3D systems with complex geometries and programmable mechanical properties. However, available micro‐origami systems usually have slow folding speeds, provide few active degrees of freedom, rely on environmental stimuli for actuation, and allow for either elastic or plastic folding but not both. This work introduces an integrated fabrication–design–actuation methodology of an electrothermal micro‐origami system that addresses the above‐mentioned challenges. Controllable and localized Joule heating from electrothermal actuator arrays enables rapid, large‐angle, and reversible elastic folding, while overheating can achieve plastic folding to reprogram the static 3D geometry. Because the proposed micro‐origami do not rely on an environmental stimulus for actuation, they can function in different atmospheric environments and perform controllable multi‐degrees‐of‐freedom shape morphing, allowing them to achieve complex motions and advanced functions. Combining the elastic and plastic folding enables these micro‐origami to first fold plastically into a desired geometry and then fold elastically to perform a function or for enhanced shape morphing. The proposed origami systems are suitable for creating medical devices, metamaterials, and microrobots, where rapid folding and enhanced control are desired.     

Metal Organic Framework-MXene Nanoarchitecture for Fast Responsive and Ultra-Stable Electro-Ionic Artificial Muscles

Electro-ionic soft actuators, capable of continuous deformations replacing non-compliant rigid mechanical components, attract increasing interest in the field of next-generation metaverse interfaces and soft robotics. Here, a novel MXene (Ti₃C₂T_x) electrode anchoring manganese-based 1,3,5-benzenetricarboxylate metal-organic framework (MnBTC) for ultrastable electro-ionic artificial muscles is reported. By a facile supramolecular self-assembly, the Ti₃C₂T_x-MnBTC hybrid nanoarchitecture forms coordinate bond, hydrogen bond, and hydrophilic interaction with the conducting polymer of poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), resulting in a mechanically flexible and electro-ionically active electrode. The superior electrical and electrochemical performances of the electrode stem from the synergistic effects between intrinsically hierarchical nanoarchitecture of MnBTC and rapid electron transport behavior of Mxene, leading to fast diffusion and accommodation of ions in the ion-exchangeable membrane. The developed artificial muscle based on Ti₃C₂T_x-MnBTC is found to exhibit high bending displacement (12.5 mm) and ultrafast response time (0.77 s) under a low driving voltage (0.5 V), along with wide frequency response (0.1–10 Hz) and exceptional stability (98% retention at 43,200 s) without any distortion of actuation performance. Furthermore, the designed electro-active artificial muscle is successfully used to demonstrate mimicry of eye motions including eyelid blinking and eyeball movement in a doll.     

Strontium Barium Niobate as a Multifunctional Two‐Dimensional Nonlinear “Photonic Glass”

The ability of Strontium Barium Niobate crystal as a two‐dimensional nonlinear optical multiple‐wavelength‐and‐direction converter is demonstrated, showing how harmonic generation can be obtained in an extremely large spectral range. The whole visible spectral region can be continuously generated without any angle or temperature tuning by using different nonlinear schemes involving SHG and THG in different configurations. The dominant frequency conversion mechanisms acting in each case are experimentally determined. The system can act as a nonlinear prism since the SHG conical radiation from 430 to 680 nm can be dispersed into an external angle range of 36°. Conical nonlinear processes are also demonstrated under intracavity conditions from a diode pumped Nd³⁺:SBN laser crystal. Different harmonic generated rings appear simultaneously inside the cavity, while the crystal is lasing at 1063 nm. The system constitutes the first experimental example of a two‐dimensional generalized nonlinear photonic glass on a tunable solid state laser and can be useful for novel optical multifunctional devices such as nonlinear prism self‐frequency converted solid state lasers.     

Self‐Propelled 3D‐Printed “Aircraft Carrier” of Light‐Powered Smart Micromachines for Large‐Volume Nitroaromatic Explosives Removal

Self‐propelled micro‐/nanomotors are in the forefront of materials research, for applications ranging from environmental remediation to biomedicine. However, due to their limited sizes, they can only navigate within small distances, typically in the order of millimeters, which inevitably hinder their use for large‐volume real applications. Here it is shown that a 3D‐printed millimeter‐scale motor (3DP‐motor) can act as “aircraft carrier” of TiO₂/Pt Janus micromotors and be used for enhanced large‐volume environmental remediation applications. The 3DP‐motor can move fast for tens of meters through the Marangoni effect by asymmetrically releasing ethanol. During its navigation, this 3DP‐motor can carry and slowly release in solution TiO₂/Pt Janus micromotors which can be propelled by light illumination while acting as photodegradation agents. Highly efficient degradation of nitroaromatic explosives over a large solution area is achieved. A wall‐following motion of the 3DP‐motor without external guidance is also demonstrated which is generated by the chemiosmotic flow at the wall vicinity. This can be easily tuned by changing the wettability of the wall surface and also modifying the shape of 3DP‐motor, leading to different motion behaviors. This work introduces a new concept of micromotors carried by large millimeter sized motors to traverse long distances and it should find a broad range of applications.     

Collectively Exhaustive Electrodes Based on Covalent Organic Framework and Antagonistic Co‐Doping for Electroactive Ionic Artificial Muscles

In this study, high‐performance ionic soft actuators are developed for the first time using collectively exhaustive boron and sulfur co‐doped porous carbon electrodes (BS‐COF‐Cs), derived from thiophene‐based boronate‐linked covalent organic framework (T‐COF) as a template. The one‐electron deficiency of boron compared to carbon leads to the generation of hole charge carriers, while sulfur, owing to its high electron density, creates electron carriers in BS‐COF‐C electrodes. This antagonistic functionality of BS‐COF‐C electrodes assists the charge‐transfer rate, leading to fast charge separation in the developed ionic soft actuator under alternating current input signals. Furthermore, the hierarchical porosity, high surface area, and synergistic effect of co‐doping of the BS‐COF‐Cs play crucial roles in offering effective interaction of BS‐COF‐Cs with poly(3,4‐ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS), leading to the generation of high electro‐chemo‐mechanical performance of the corresponding composite electrodes. Finally, the developed ionic soft actuator based on the BS‐COF‐C electrode exhibits large bending strain (0.62%), excellent durability (90% retention for 6 hours under operation), and 2.7 times higher bending displacement than PEDOT:PSS under extremely low harmonic input of 0.5 V. This study reveals that the antagonistic functionality of heteroatom co‐doped electrodes plays a crucial role in accelerating the actuation performance of ionic artificial muscles.     

“Black” Titania Coatings Composed of Sol–Gel Imprinted Mie Resonators Arrays

Optical technologies and devices rely on the controlled manipulation of light propagation through a medium. This is generally governed by the inherent effective refractive index of the material as well as by its structure and dimensionality. Although a precise control over light propagation with sub‐wavelength size objects is a crucial issue for a plethora of applications, the widely used fabrication methods remain cumbersome and expensive. Here, a sol–gel dip‐coating method combined with nanoimprinting lithography on arbitrary glass and silicon substrates is implemented for the fabrication of TiO₂‐based dielectric Mie resonators. The technique allows obtaining sub‐micrometric pillars featuring unprecedented vertical aspect ratios (>1) with relatively high fidelity and precision. Spectroscopic characterization at visible and near‐infrared frequencies demonstrate that the resonant properties of these dielectric pillar arrays allow for a drastic reduction of light transmission (cutting more than 50% on glass) and reduced reflection (reflecting less than 3% on glass and 16% on bulk silicon), accounting for an efficient light trapping. These results provide a guideline for the fabrication of Mie resonators using a fast, versatile, low‐cost, low‐temperature technique for efficient light manipulation at the nanoscale.     

Stability and Hydrogenation of “Bare” Gadolinium Nanoparticles

Gadolinium nanoparticles, deposited via an inert gas evaporation method, show improved stability towards oxidation and it is therefore possible to carry out an ex‐situ investigation on “bare” Gd nanoparticles, i.e., in the absence of a protective Pd layer, for the first time. A size‐induced structural transformation from hexagonal close packing to the higher‐symmetry face‐centered cubic structure is observed. The important observation of hydrogen–Gd‐nanoparticle interaction at room temperature and atmospheric pressure, without a Pd catalytic layer, makes Gd nanoparticles a potential candidate for hydrogen‐sensing, switching, and storage applications.     

Superhydrophobic “Pump”: Continuous and Spontaneous Antigravity Water Delivery

Antigravity transportation of water, which is often observed in nature, is becoming a vital demand for advanced devices and new technology. Many studies have been devoted to the motion of a single droplet on a horizontal or inclined substrate under specific assistance. However, the self‐propelled water motion, especially continuous antigravity water delivery, still remains a considerable challenge. Here, a novel self‐ascending phenomenon driven only by the surface energy release of water droplets is found, and a superhydrophobic mesh to pump water up to a height of centimeter scale is designed. An integrated antigravity transportation system is also demonstrated to continuously and spontaneously pump water droplets without additional driving forces. The present novel finding and integrated devices should serve as a source of inspiration for the design of advanced materials and for the development of new technology with exciting applications in microfluidics, microdetectors, and intelligent systems.     

Harnessing “Click”‐Type Chemistry for the Preparation of Novel Electronic Materials

Sequence‐independent or “click”‐type chemistry is applied for the preparation of novel π‐conjugated oligomers. A variety of bi‐functional monomers for Wittig–Horner olefination are developed and applied in a sequential protection–deprotection process for the preparation of structurally similar π‐conjugated oligomers. Selected oligomers are incorporated as the organic semiconductors in light‐emitting diodes and a field‐effect transistor, demonstrating the potential of the approach.     

Bio‐Inspired All‐Organic Soft Actuator Based on a π–π Stacked 3D Ionic Network Membrane and Ultra‐Fast Solution Processing

Next generation electronic products, such as wearable electronics, flexible displays, and smart mobile phones, will require the use of unprecedented electroactive soft actuators for haptic and stimuli‐responsive devices and space‐saving bio‐mimetic actuation. Here, a bio‐inspired all‐organic soft actuator with a π–π stacked and 3D ionic networked membrane based on naphthalene‐tetracarboxylic dianhydride (Ntda) and sulfonated polyimide block copolymers (SPI) is presented, utilizing an ultra‐fast solution process. The π–π stacked and self‐assembled 3D ionic networked membrane with continuous and interconnected ion transport nanochannels is synthesized by introducing simple and strong atomic level regio‐specific interactions of hydrophilic and hydrophobic SPI co‐blocks with cations and anions in the ionic liquid. Furthermore, a facile and ultrafast all‐solution process involving solvent blending, dry casting, and solvent dropping is developed to produce electro‐active soft actuators with highly conductive polyethylenedioxythiophene (PEDOT):polystyrenesulfonate (PSS) electrodes. Ionic conductivity and ion exchange capacity of the π–π stacked Ntda‐SPI membrane can be increased up to 3.1 times and 3.4 times of conventional SPI, respectively, resulting in a 3.2 times larger bending actuation. The developed bio‐inspired soft actuator is a good candidate for satisfying the tight requirements of next generation soft electronic devices due to its key benefits such as low operating voltage and comparatively large strains, as well as quick response and facile processability.     

Machine Learning‐Enabled Correlation and Modeling of Multimodal Response of Thin Film to Environment on Macro and Nanoscale Using “Lab‐on‐a‐Crystal”

To close the feedback loop between artificial intellegence‐controlled materials synthesis and characterization, material functionality must be rapidly tested. A platform for high‐throughput multifunctional materials characterization is developed using a quartz crystal microbalance with auxiliary in‐plane electrodes and a custom gas/vapor flow cell, enabling simultaneous scanning probe microscopy and electrical, optical, gravimetric, and viscoelastic characterization on the same film under controlled environment. The lab‐on‐a‐crystal in situ multifunctional output allows direct correlations between the gravimetric/viscoelastic, electrical, and optical responses of polymer film in response to environment. When multiple film properties are used to augment the training set for machine learning regression, prediction of material response to the environment improves by a factor of 13 when <5% of the total dataset is used for model training.     

“MeshUp”: Self-organizing mesh-based topologies for next generation radio access networks

The phenomenal growth in wireless technologies has brought about a slew of new services. Incumbent with the new technology is the challenge of providing flexible, reconfigurable, self-organizing architectures which are capable of catering to the dynamics of the network, while providing cost-effective solutions for the service providers. In this paper, we focus on mesh-based multi-hop access network architectures for next generation radio access networks. Using short, high bandwidth optical wireless links to interconnect the various network elements, we propose a non-hierarchical, multi-hop access network framework. We study two generic family of mesh-based topologies: GPeterNet, a graph theoretic framework, and FraNtiC, a fractal geometric architecture, for arbitrary access network deployments. The performance of these topologies is analyzed in terms of different system metrics – topological robustness and reliability, system costs and network exposure due to failure conditions. Our analysis shows that a combination of different mesh-based multi-hop access topologies, coupled with emerging wireless backhaul technologies, can cater carrier-class services for next generation radio access networks, providing significant advantages over existing access technologies.     

A “Group-Division Multiple Access” framework for channel access to multiple destinations

We consider the problem of media-access control in multiple-cell networks, such as ad hoc networks in which clusterheads take on a role similar to base stations. We assume that a single channel is used by all cells, and that the user populations that transmit to different base stations overlap, causing interference in the neighboring cells. Starting with a two-destination network, we introduce the “Group-Division Multiple Access” (GDMA) concept, according to which different groups of users multiplex their transmission in time while being free to use the protocol of their choice within their own group. We show that use of GDMA provides higher stable throughput than a “free-running” scheme (under which all slots are available to all users) when the First-Come First-Serve collision–resolution algorithm is used as the channel-access protocol, and we show how performance depends on the degree of overlap of communication and interference regions. Finally, we show that this approach can be applied to larger cellular-like networks as well.     

Conductive “Smart” Hybrid Hydrogels with PNIPAM and Nanostructured Conductive Polymers

Stimuli‐responsive hydrogels with decent electrical properties are a promising class of polymeric materials for a range of technological applications, such as electrical, electrochemical, and biomedical devices. In this paper, thermally responsive and conductive hybrid hydrogels are synthesized by in situ formation of continuous network of conductive polymer hydrogels crosslinked by phytic acid in poly(N‐isopropylacrylamide) matrix. The interpenetrating binary network structure provides the hybrid hydrogels with continuous transporting path for electrons, highly porous microstructure, strong interactions between two hydrogel networks, thus endowing the hybrid hydrogels with a unique combination of high electrical conductivity (up to 0.8 S m^?1), high thermoresponsive sensitivity (significant volume change within several seconds), and greatly enhanced mechanical properties. This work demonstrates that the architecture of the filling phase in the hydrogel matrix and design of hybrid hydrogel structure play an important role in determining the performance of the resulting hybrid material. The attractive performance of these hybrid hydrogels is further demonstrated by the developed switcher device which suggests potential applications in stimuli‐responsive electronic devices.     

A “Trojan Horse” Camouflage Strategy for High‐Performance Cellulose Paper and Separators

Lignin‐carbohydrate complexes (LCC) underpin the comprehensive properties of natural wood. Facile restoration of LCC analogues in paper is challenging because of the charge repulsion between negatively charged lignin and pulp fibrils. A camouflage strategy is discovered to prepare positively charged lignosulfonate–polyamide‐epichlorohydrin complex (LPC) nanoparticles, which are effectively incorporated in pulp through the “LPC–pulp” attraction instead of “lignosulfonate–pulp” repulsion. Water‐resistant LPC paper sheets are prepared in ≈20 min without pressurization. They exhibit high tensile strength (41 MPa), surviving boiling water treatment for 14 days, on par with the strength of pristine paper and certain plastics in a dry state. The camouflage strategy applies to various pulps and processing technologies, as exemplified by a paper separator showing exceptional electrolyte wettability and rate capability in lithium‐ion batteries. This work establishes advanced cellulose valorization with combined strength, water stability, and tailored microstructures replacing petroleum polymers in engineering and energy implications.     

Adaptations for Wear Resistance and Damage Resilience: Micromechanics of Spider Cuticular “Tools”

In the absence of minerals as stiffening agents, insects and spiders often use metal‐ion cross‐linking of protein matrices in their fully organic load‐bearing “tools.” In this comparative study, the hierarchical fiber architecture, elemental distribution, and the micromechanical properties of the manganese‐ and calcium‐rich cuticle of the claws of the spider Cupiennius salei, and the Zn‐rich cuticle of the cheliceral fangs of the same animal are analyzed. By correlating experimental results to finite element analysis, functional microstructural and compositional adaptations are inferred leading to remarkable damage resilience and abrasion tolerance, respectively. The results further reveal that the incorporation of both zinc and manganese/calcium correlates well with increased biomaterial's stiffness and hardness. However, the abrasion‐resistance of the claw material cross‐linked by incorporation of Mn/Ca‐ions surpasses that of many other non‐mineralized biological counterparts and is comparable to that of the fang with more than triple Zn content. These biomaterial‐adaptation paradigms for enhanced wear‐resistance may serve as novel design principles for advanced, high‐performance, functional surfaces, and graded materials.