Bioinspired Continuous and Spontaneous Antigravity Oil Collection and Transportation

Liquids with low surface tension, such as petroleum, serve as the source of power for development of modern industry. Spontaneous and directional transportation of oily liquids in aqueous environment has drawn wide attentions owing to its scientific significance and practical prospect in marine petroleum exploitation and oil spill cleanup. Persistent effort has been made to the directional transportation of oil droplets under specific assistance. However, the spontaneous oriented movement of oil, especially the air/water two‐phase oil delivery is still identified as a big challenge. Here, a bioinspired superoleophobic pump has been fabricated through the assembly of a superoleophobic mesh and an oil column. Depending on the directional releases of surface energy, oil droplets can be continuously collected and pumped to centimeters high without additional driving forces. The antigravity oil delivery system can realize continuous oil flow under water, even the air/water two‐phase oil transportation. This work demonstrates a new mode of liquid transportation without external energy and should open a new way to design novel fluid delivery systems to realize diverse liquid transport.     

Droplet‐Based Self‐Propelled Miniboat

Self‐propelled autonomous devices have huge application prospects in the field of environmental protection and energy. Nonetheless, the requirement of special chemicals or external electric and thermal energy limits their practical application. Here, a green self‐propelling method based on Laplace pressure originated from water droplets is reported. First, a triangle‐shaped miniboat composed of a superhydrophobic plate with an inclined superhydrophilic pore is fabricated. Water droplets put on superhydrophilic pore pass through the pore and form a jellyfish‐like jet, which further propels the miniboat to move spontaneously and directionally. The propelling distance, propelling time, and instantaneous propelling velocity of the miniboat is greatly affected by the pore size and the initial water droplet volume. Then, two types of devices are designed and installed on the miniboat to successively provide small water droplets from the reservoir or rain to realize the continuous and long‐distance self‐propelled motion. Moreover, a spindle‐shaped miniboat with two or four symmetrical and inclined pores is designed. Under propelling by the torque, the spontaneous and continuous rotation motion is also achieved. This finding will open a new avenue for a wide range of applications ranging from a detecting minirobot on the water surface to a power generation device from rain.     

Simultaneous “Clean‐and‐Repair” of Surfaces Using Smart Droplets

An autonomous self‐healing system, inspired by transportation processes inherent to biology, is described for materials transportation and repair. The selected model system combines inorganic nanoparticles (NPs) on damaged substrates with functional emulsion droplets that pick up the particles from pristine portions of the substrate and deposit them into damaged regions. The droplets are stabilized by polymer surfactants containing phosphorylcholine groups, a polymer composition selected to impart surfactant properties for droplet stabilization as well as fouling resistance to prevent irreversible droplet adsorption on the substrates. Both the NP pickup (cleaning) and drop off (repair) steps are conducted in a system driven by an imposed flow and characterized by fluorescence microscopy. To evaluate and optimize the efficiency of this NP transportation process, the effect of both the chemical composition of the polymer surfactant and the NP surface chemistry is investigated. Interfacial interactions proved enabling for these NP transportation processes, specifically those involving NP/droplet, NP/substrate, and droplet/substrate interactions. Ultimately, droplets capable of both picking up and dropping off NPs are realized by adjusting fluid/fluid and fluid/substrate interactions, with electrostatic interactions between NPs and droplets proving most effective.     

Bio‐Inspired Anisotropic Wettability Surfaces from Dynamic Ferrofluid Assembled Templates

The biomimetic principle of harnessing topographical structures to determine liquid motion behavior represents a cutting‐edge direction in constructing green transportation systems without external energy input. Here, inspired by natural Nepenthes peristome, a novel anisotropic wettability surface with characteristic structural features of periodically aligned and overlapped arch‐shaped microcavities, formed by employing ferrofluid assemblies as dynamic templates, is presented. The magnetic strength and orientation are precisely adjustable during the generation process, and thus the size and inclination angle of the ferrofluid droplet templates could be tailored to make the surface morphology of the resultant polymer replica achieve a high degree of similarity to the natural peristome. The resultant anisotropic wettability surface enables autonomous unidirectional water transportation in a fast and continuous way. In addition, it could be tailored into arbitrary shapes to induce water flow along a specific curved path. More importantly, based on the anisotropic wettability surface, novel pump‐free microfluidic devices are constructed to implement multiphase flow reactions, which offer a promising solution to building low‐cost, portable platform for lab‐on‐a‐chip applications.     

Molecular Engineering of “Click”‐Phospholes Towards Self‐Assembled Luminescent Soft Materials

Inspired by the self‐assembled bilayer structures of natural amphiphilic phospholipids, a new class of highly luminescent “click”‐phospholes with exocyclic alkynyl group at the phosphorus center is reported. These molecules can be easily functionalized with a self‐assembly group to generate neutral “phosphole‐lipids”. This novel approach retains the versatile reactivity of the phosphorus center, allowing further engineering of the photophysical and self‐assembly properties of the materials at a molecular level. The results of this study highlight the importance of being able to balance weak intermolecular interactions for controlling the self‐assembly properties of soft materials. Only molecules with the appropriate set of intermolecular arrangement/interactions show both organogel and liquid crystal mesophases with well‐ordered microstructures. Moreover, an efficient energy transfer of the luminescent materials is demonstrated and applied in the detection of organic solvent vapors.     

All‐Solution‐Processed Cu2ZnSnS4 Solar Cells with Self‐Depleted Na2S Back Contact Modification Layer

The thin‐film photovoltaic material Cu₂ZnSnS₄ (CZTS) has drawn worldwide attention in recent years due to its earth‐abundant, nontoxic element constitution, and remarkable photovoltaic performance. Although state‐of‐the‐art power conversion efficiency is achieved by hydrazine‐based methods, effort to fabricate such devices in a high throughput, environmental‐friendly way is still highlydesired. Here a hydrazine‐free all‐solution‐processed CZTS solar cell with Na₂S self‐depleted back contact modification layer for the first time is demonstrated, using a ball‐milled CZTS as light absorber, low‐temperature solution‐processed ZnO electron‐transport layer as well as silver‐nanowire transparent electrode. The inserting of Na₂S self‐depleted layer is proven to effectively stabilize the CZTS/Mo interface by eliminating a detrimental phase segregation reaction between CZTS and Mo‐coated soda lime glass, thus leading to a better crystallinity of CZTS light absorbing layer, enhanced carrier transportation at CZTS/Mo interface as well as a smaller series resistance. Furthermore, the self‐depletion feature of the Na₂S modification layer also averts hole‐transportation barrier within the devices. The results show the vital importance of interfacial engineering for these CZST devices and the Na₂S interface layer can be extended to other optoelectronic devices using Mo contact.     

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.     

Self‐Powered Noncontact Electronic Skin for Motion Sensing

The advancement of electronic skin envisions novel multifunctional human machine interfaces. Although motion sensing by detecting contact locations is popular and widely used in state‐of‐the‐art flexible electronics, noncontact localization exerts fascinations with unique interacting experiences. This paper presents a self‐powered noncontact electronic skin capable of detecting the motion of a surface electrified object across the plane parallel to that of the electronic skin based on electrostatic induction and triboelectric effects. The displacement of the object is calculated under the system of polar coordinates, with a resolution of 1.5 mm in the lengthwise direction and 0.76° in the angular direction. It can serve as a human machine interface due to its ability to sense noncontact motions. An additional self‐powered feature, enabled by its physical principles, solves the problem of power supply. This electronic skin consists of trilayers of polyethyleneterephthalate–indium tin oxide–polydimethylsiloxane (PDMS) films, and microstructured PDMS as the electrified layer, which can be achieved through simplified, low cost, and scalable fabrication. Transparency, flexibility, and less number of electrodes enable such electronic skin to be easily integrated into portable electronic devices, such as laptops, smart phones, healthcare devices, etc.     

Self‐Healing,Flexible, and Tailorable Triboelectric Nanogenerators for Self‐Powered Sensors based on Thermal Effect of Infrared Radiation

Self‐healing triboelectric nanogenerators (TENGs) with flexibility, robustness, and conformability are highly desirable for promising flexible and wearable devices, which can serve as a durable, stable, and renewable power supply, as well as a self‐powered sensor. Herein, an entirely self‐healing, flexible, and tailorable TENG is designed as a wearable sensor to monitor human motion, with infrared radiation from skin to promote self‐healing after being broken based on thermal effect of infrared radiation. Human skin is a natural infrared radiation emitter, providing favorable conditions for the device to function efficiently. The reversible imine bonds and quadruple hydrogen bonding (UPy) moieties are introduced into polymer networks to construct self‐healable electrification layer. UPy‐functionalized multiwalled carbon nanotubes are further incorporated into healable polymer to obtain conductive nanocomposite. Driven by the dynamic bonds, the designed and synthesized materials show excellent intrinsic self‐healing and shape‐tailorable features. Moreover, there is a robust interface bonding in the TENG devices due to the similar healable networks between electrification layer and electrode. The output electric performances of the self‐healable TENG devices can almost restore their original state when the damage of the devices occurs. This work presents a novel strategy for flexible devices, contributing to future sustainable energy and wearable electronics.     

Ultrahigh‐Performance Flexible and Self‐Powered Photodetectors with Ferroelectric P(VDF‐TrFE)/Perovskite Bulk Heterojunction

Flexible and self‐powered perovskite photodetectors attract widespread research interests due to their potential applications in portable and wearable optoelectronic devices. However, the reported devices mainly adopt an independent layered structure with complex fabrication processes and high carrier recombination. Herein, an integrated ferroelectric poly(vinylidene‐fluoride‐trifluoroethylene) (P(VDF‐TrFE)) and perovskite bulk heterojunction film photodetector on the polyethylene naphthalate substrate is demonstrated. Under the optimum treatment conditions (the polarization voltage and time, and the concentration of P(VDF‐TrFE)), the photodetector exhibits a largely enhanced performance compared to the pristine perovskite device. The resulting device exhibits ultrahigh performance with a large detectivity (1.4 × 10¹³ Jones) and fast response time (92/193 µs) at the wavelength of 650 nm. The improved performance is attributed to the fact that the polarized P(VDF‐TrFE)/perovskite hybrid film provides a stronger built‐in electric field to facilitate the separation and transportation of photogenerated carriers. These findings provide a new route to design self‐powered photodetectors from the aspect of device structure and carrier transport.     

Removal of Microparticles by Ciliated Surfaces—an Experimental Study

Biological cilia are versatile hair‐like organelles that are very efficient in manipulating particles for, e.g., feeding, antifouling, and cell transport. Inspired by the versatility of cilia, this paper experimentally demonstrates active particle‐removal by self‐cleaning surfaces that are fully or partially covered with micromolded magnetic artificial cilia (MAC). Actuated by a rotating magnet, the MAC can perform a tilted conical motion, which leads to the removal of spherical particles of different sizes in water, as well as irregular‐shaped sand grains both in water and in air. These findings can contribute to the development of novel particulate manipulation and self‐cleaning/antifouling surfaces, which can be applied, e.g., to prevent fouling of (bio)sensors in lab‐on‐a‐chip devices, and to prevent biofouling of submerged surfaces such as marine sensors and water quality analyzers.     

A Highly Stretchable Fiber‐Based Triboelectric Nanogenerator for Self‐Powered Wearable Electronics

The development of flexible and stretchable electronics has attracted intensive attention for their promising applications in next‐generation wearable functional devices. However, these stretchable devices that are made in a conventional planar format have largely hindered their development, especially in highly stretchable conditions. Herein, a novel type of highly stretchable, fiber‐based triboelectric nanogenerator (fiber‐like TENG) for power generation is developed. Owing to the advanced structural designs, including the fiber‐convolving fiber and the stretchable electrodes on elastic silicone rubber fiber, the fiber‐like TENG can be operated at stretching mode with high strains up to 70% and is demonstrated for a broad range of applications such as powering a commercial capacitor, LCD screen, digital watch/calculator, and self‐powered acceleration sensor. This work verifies the promising potential of a novel fiber‐based structure for both power generation and self‐powered sensing.     

Genesis of “Solitary Cations” Induced by Atomic Hydrogen

Substitution of constituent atoms and/or changes of crystal structure are routinely used to tailor the fundamental properties of a semiconductor. Here, it is shown that such a tailoring can also be realized thanks to a novel hydrogen effect. Four hydrogen atoms can screen the effect the crystal potential has on a constituent cation, thus generating a solitary cation: an effectively isolated impurity, so chemically different from the unscreened constituent cations that it strongly perturbs the electronic properties of the material by increasing its fundamental band‐gap energy. Such a hydrogen‐induced screening effect is removed by thermal treatments, thus permitting reversible modifications of both the “crystal chemistry” and material's properties. This phenomenon, observed in InN and other topical nitrides, should permit the development of a new class of materials as well as the fabrication of photonic devices and optical integrated circuits with distinct, tailor‐made regions emitting or absorbing light, all integrated onto a monolithic semiconductor structure.     

Remote Steering of Self‐Propelling Microcircuits by Modulated Electric Field

The principles and design of “active” self‐propelling particles that can convert energy, move directionally on their own, and perform a certain function is an emerging multidisciplinary research field, with high potential for future technologies. A simple and effective technique is presented for on‐demand steering of self‐propelling microdiodes that move electroosmotically on water surface, while supplied with energy by an external alternating (AC) field. It is demonstrated how one can control remotely the direction of diode locomotion by electronically modifying the applied AC signal. The swimming diodes change their direction of motion when a wave asymmetry (equivalent to a DC offset) is introduced into the signal. The data analysis shows that the ability to control and reverse the direction of motion is a result of the electrostatic torque between the asymmetrically polarized diodes and the ionic charges redistributed in the vessel. This novel principle of electrical signal‐coded steering of active functional devices, such as diodes and microcircuits, can find applications in motile sensors, MEMs, and microrobotics.     

Droplets Crawling on Peristome‐Mimetic Surfaces

Controlling the mobility of liquids along surfaces is widely exploited in various technologies to achieve self‐lubrication, phase‐change heat transfer, and microfluidics. Despite commendable progress in directional liquid transport on peristome‐mimetic surfaces, liquid merely spreads directionally with a wetted trail remaining. It is a challenge to achieve directional contracting of spreading liquid at the rear side and ultimately unidirectional motion in bulk from one site to another. Here it is shown that liquids resting on the peristome‐mimetic surfaces can crawl directionally and rapidly in an inchworms‐like way under the action of sudden spontaneous bubbles levitation. Vacuuming or chemical reaction induces sudden nucleation, growth, coalescence (Ostwald ripening process), and rupture of bubbles in the asymmetric microcavities of the peristome‐mimetic surface with directional overpressure beneath the liquid, resulting in the guided contracting and spreading of the liquid. Bubbles regulate this new mode of liquid directional motion. The strategy offers opportunities for liquids directional motion for various applications, such as in microfluidic devices, oil–water separation, and water collection systems.     

Magnetic Liquid Marbles: Toward “Lab in a Droplet”

Liquid marbles exhibit great potential for use as miniature labs for small‐scale laboratory operations, such as experiment and measurement. While important progress has been made recently in exploring their applications as microreactions, “on‐line” measurement of the components inside the liquid still remains a challenge. Herein, it is demonstrated that “on‐line” detection can be realized on magnetic liquid marbles by taking advantage of their unique magnetic opening feature. By partially opening the particle shell, electrochemical measurement is carried out with a miniaturized three‐electrode probe and the application of this technique for quantitative measurement of dopamine is demonstrated. Fully opened magnetic liquid marble makes it feasible to detect the optical absorbance of the liquid in a transmission mode. With this optical method, a glucose assay is demonstrated. Moreover, when magnetic particle shell contains low melting point material, e.g., wax, the liquid marble shows a unique encapsulation ability to form a rigid shell after heating, which facilitates the storage of the non‐volatile ingredients. These unique features, together with the versatile use as microreactors, enable magnetic liquid marbles to function as a miniature lab (or called “lab in a droplet”), which may find applications in clinical diagnostics, biotechnology, chemical synthesis, and analytical chemistry.     

Controllable Stiffness Origami “Skeletons” for Lightweight and Multifunctional Artificial Muscles

Flexible, material‐based, artificial muscles enable compliant and safe technologies for human–machine interaction devices and adaptive soft robots, yet there remain long‐term challenges in the development of artificial muscles capable of mimicking flexible, controllable, and multifunctional human activity. Inspired by human limb's activity strategy, combining muscles' adjustable stiffness and joints' origami folding, controllable stiffness origami “skeletons,” which are created by laminar jamming and origami folding of multiple layers of flexible sandpaper, are embedded into a common monofunctional vacuumed‐powered cube‐shaped (CUBE) artificial muscle, thereby enabling the monofunctional CUBE artificial muscle to achieve lightweight and multifunctionality as well as controllable force/motion output without sacrificing its volume and shape. Successful demonstrations of arms self‐assembly and cooperatively gripping different objects and a “caterpillar” robot climbing different pipes illustrate high operational redundancy and high‐force output through “building blocks” assembly of multifunctional CUBE artificial muscles. Controllable stiffness origami “skeletons” offer a facile and low‐cost strategy to fabricate lightweight and multifunctional artificial muscles for numerous potential applications such as wearable assistant devices, miniature surgical instruments, and soft robots.     

Multi‐“Color” Delineation of Bone Microdamages Using Ligand‐Directed Sub‐5 nm Hafnia Nanodots and Photon Counting CT Imaging

The early detection of bone microdamages is crucial to make informed decisions about the therapy and taking precautionary treatments to avoid catastrophic fractures. Conventional computed tomography (CT) imaging faces obstacles in detecting bone microdamages due to the strong self‐attenuation of photons from bone and poor spatial resolution. Recent advances in CT technology as well as novel imaging probes can address this problem effectively. Herein, the bone microdamage imaging is demonstrated using ligand‐directed nanoparticles in conjunction with photon counting spectral CT. For the first time, Gram‐scale synthesis of hafnia (HfO₂) nanoparticles is reported with surface modification by a chelator moiety. The feasibility of delineating these nanoparticles from bone and soft tissue of muscle is demonstrated with photon counting spectral CT equipped with advanced detector technology. The ex vivo and in vivo studies point to the accumulation of hafnia nanoparticles at microdamage site featuring distinct spectral signal. Due to their small sub‐5 nm size, hafnia nanoparticles are excreted through reticuloendothelial system organs without noticeable aggregation while not triggering any adverse side effects based on histological and liver enzyme function assessments. These preclinical studies highlight the potential of HfO₂‐based nanoparticle contrast agents for skeletal system diseases due to their well‐placed K‐edge binding energy.     

Hybrid Smart Fiber with Spontaneous Self‐Charging Mechanism for Sustainable Wearable Electronics

Smart wearable electronics that are fabricated on light‐weight fabrics or flexible substrates are considered to be of next‐generation and portable electronic device systems. Ideal wearable and portable applications not only require the device to be integrated into various fiber form factors, but also desire self‐powered system in such a way that the devices can be continuously supplied with power as well as simultaneously save the acquired energy for their portability and sustainability. Nevertheless, most of all self‐powered wearable electronics requiring both the generation of the electricity and storing of the harvested energy, which have been developed so far, have employed externally connected individual energy generation and storage fiber devices using external circuits. In this work, for the first time, a hybrid smart fiber that exhibits a spontaneous energy generation and storage process within a single fiber device that does not need any external electric circuit/connection is introduced. This is achieved through the employment of asymmetry coaxial structure in an electrolyte system of the supercapacitor that creates potential difference upon the creation of the triboelectric charges. This development in the self‐charging technology provides great opportunities to establish a new device platform in fiber/textile‐based electronics.     

Hydrophilic/Oleophilic Magnetic Janus Particles for the Rapid and Efficient Oil–Water Separation

The separation of microsized oil droplets from water is strongly required by the environmental protection and petroleum industry. However, the separation of microsized oil droplets from water is often ignored. Herein, magnetic Janus particles are reported with a convex hydrophilic surface/concave oleophilic surface by emulsion interfacial polymerization and selective surface assembly, realizing the rapid and efficient separation of microscaled tiny oil droplets from water. These magnetic Janus particles exhibit significant abilities to separate microscaled oil droplets from water, which usually occurs within 120 s with a separation efficiency >99%. Theoretical and experimental results demonstrate that these magnetic Janus particles can capture tiny oil droplets to make them coalesce into larger ones during the process of separation. Further studies reveal that these Janus particles can self‐assemble and closely pack onto the interface of larger oil droplets, acting as surfactants to stabilize them. Moreover, the shape effect of the Janus particle is demonstrated on the coalescence of the oil droplets.