Soft Materials Research Articles

Dual design strategy for carboxymethyl cellulose-polyaniline composite hydrogels as super-sensitive amphibious sensors

Conductive hydrogels as ideal candidate materials for flexible sensors have exhibited many promising applications. However, complex application environments, such as low temperatures or underwater conditions, have introduced new requirements for hydrogel sensors. Herein, a high-performance conductive hydrogel based on carboxymethyl cellulose-polyaniline (CMC-PANI) submicron spheres, poly (vinyl alcohol) (PVA) and phytic acid (PA) was designed and fabricated via a dual design strategy. CMC-PANI particles were introduced to not only empower the good electromechanical performance to the hydrogels, but also enhance the mechanical properties. The obtained hydrogel exhibited good mechanical property, anti-freezing, anti-swellable behavior and recyclable performance. Resistive-type strain sensors assembled by the prepared hydrogels exhibited high pressure sensitivity (34.17×10−2 kPa−1) and fast response time (100 ms), which can clearly detect the pulse beats. Moreover, the hydrogel sensors can achieve long-term stability, high sensitivity and fatigue resistance as an underwater sensor. Based on these favorable performances, the conductive polymer hydrogels may open up an enticing avenue for functional soft materials in health diagnostic and electronic components.

Evaluating Cryo-TEM Reconstruction Accuracy of Self-Assembled Polymer Nanostructures.

Cryogenic transmission electron microscopy (cryo-TEM) combined with single particle analysis (SPA) is an emerging imaging approach for soft materials. However, the accuracy of SPA-reconstructed nanostructures, particularly those formed by synthetic polymers, remains uncertain due to potential packing heterogeneity of the nanostructures. In this study, the combination of molecular dynamics (MD) simulations and image simulations is utilized to validate the accuracy of cryo-TEM 3D reconstructions of self-assembled polypeptoid fibril nanostructures. Using CryoSPARC software, image simulations, 2D classifications, ab initio reconstructions, and homogenous refinements are performed. By comparing the results with atomic models, the recovery of molecular details is assessed, heterogeneous structures are identified, and the influence of extraction location on the reconstructions is evaluated. These findings confirm the fidelity of single particle analysis in accurately resolving complex structural characteristics and heterogeneous structures, exhibiting its potential as a valuable tool for detailed structural analysis of synthetic polymers and soft materials.

Effect of combined treatments of hydrolysis and succinylation on the solubility and emulsion stability of rennet casein and micellar casein

Casein is the most abundant protein in milk with good emulsifying properties and bioavailability. However, the tight micellar structure of casein results in poor solubility. In the case of soft solid materials such as processed cheese, imitation cheese, yoghurt and protein-based oil-in-water emulsions, poor solubility directly affects the homogeneity and stability of the texture structure of such products, leading to a poor user experience. In this study, two protein modification techniques, hydrolysis and succinylation, were combined to improve the solubility of casein and the stability of its emulsions. The individual and combined effects of enzymatic hydrolysis and succinylation modification approaches on the stability of rennet casein (RC) and micellar casein (MC) emulsions were further explored. After double-treatment of casein with enzymatic hydrolysis and succinylation, the solubility of RC and MC was up to about 95 %, which was superior to that of single-treatment. Fourier transform infrared spectroscopy showed that the characteristic wave signals of the double-treated samples were located between the two single-treated samples, and that there may be an opposite effect between the two modifications. After 21 days of storage, the emulsions prepared from double-treated caseins still remained stable. The salt ionic stability and freeze-thaw stability were significantly improved, and the physical stability of MC was increased by nearly three times. The results explained the effects of enzymatic hydrolysis and succinylation on the functional properties of casein, provided a reference for the development of food systems based on oil-in-water emulsions, and offered a new idea for the wide application of succinylated casein.

Geometrical incompatibility regulated pattern selection and morphological evolution in growing spherical soft tissues

Surface morphological patterns are widely observed in natural systems, which are closely correlated to vital biological functions and inspire surface morphology designs in soft matter systems. Geometrical incompatibility widely exists in biological tissues across different length scales and plays an important role in growth-induced pattern selection and morphological evolution of soft tissues. However, the underlying physical mechanism of growth-induced pattern formation and post-buckling evolution in geometrically incompatible spherical soft tissues remain elusive. Here, the effect of geometrical incompatibility on the growth-induced pattern selection and post-buckling evolution are investigated through swelling experiment, theoretical analysis and numerical simulation. The results show that not only the instability pattern but also the instability threshold can be regulated by manipulating geometric incompatibility. Notably, when the geometrical incompatibility parameter exceeds a critical value, spontaneous instability is observed before growth. With continuous growth, the core–shell soft sphere buckles into a periodic buckyball pattern and evolves toward a bean-shaped pattern, and then undergoes a wrinkle-to-fold transition into a labyrinth topography. Our results demonstrate, both experimentally and theoretically, that geometrical incompatibility can guide the growth-induced pattern formation and morphological evolution effectively. This study not only enhances our understanding of the growth-induced pattern selection and morphological evolution in spherical soft tissues, but also provides an inspiring insight for the fabrication of morphological patterns on curved surfaces.

Stretchable supramolecular hydrogel with instantaneous self-healing for electromagnetic interference shielding control and sensing

Conductive hydrogels possess instantaneous self-healing and adhesive properties have generated great excitement in the fields of sensing and electromagnetic interference (EMI) shielding. In this study, we ingeniously designed hydrogel-based soft materials with high conductivity by using poly(vinyl alcohol) (PVA), positively charged Ti3C2Tx MXene and thioctic acid (TA) as source materials. Through concentration-induced ring-opening polymerization of TA monomers in an aqueous solution of potassium hydroxide (KOH), supramolecular poly(potassium thioctate) (poly(PT)) was obtained. Then, the multifunctional poly(PT)/PVA/p-MXene hydrogel with exceptional stretchability, substrate-adhesion and self-healing capability was achieved through abundant dynamic bonds, including disulfide bonds, hydrogen bonds, coordination bonds and electrostatic interactions. The hydrophobic main chains within poly(PT) provide robust protection against the oxidative degradation of MXene. This hydrogel shows outstanding strain sensing and extraordinary EMI shielding effectiveness (SE) of 48.56 dB caused by the inner structure, conductivity, and water content. Interestingly, the EMI SE can be regulated by reabsorbing moisture from the air, thereby enabling the reuse of dried hydrogel. Furthermore, the EMI SE can be dynamically modulated through controlled deformations, confirming the potential application for electromagnetic waves (EMWs) sensing. This innovative approach not only simplifies the fabrication of multifunctional materials but also expands the applications of adhesive hydrogels with conductivity.

Fabrication of Flexible Wearable Mechanosensors Utilizing Piezoelectric Hydrogels Mechanically Enhanced by Dipole-Dipole Interactions.

Conductive hydrogels have been increasingly employed to construct wearable mechanosensors due to their excellent mechanical flexibility close to that of soft tissues. In this work, piezoelectric hydrogels are prepared through free radical copolymerization of acrylamide (AM) and acrylonitrile (AN) and further utilized in assembling flexible wearable mechanosensors. Introduction of the polyacrylonitrile (PAN) component in the copolymers endows the hydrogels with excellent piezoelectric properties. Meanwhile, significant enhancement of mechanical properties has been accessed by forming dipole-dipole interactions, which results in a tensile strength of 0.51 MPa. Flexible wearable mechanosensors are fabricated by utilizing piezoelectric hydrogels as key signal converting materials. Self-powered piezoelectric pressure sensors are assembled with a sensitivity (S) of 0.2 V kPa-1. Additionally, resistive strain sensors (gauge factor (GF): 0.84, strain range: 0-250%) and capacitive pressure sensors (S: 0.23 kPa-1, pressure range: 0-8 kPa) are fabricated by utilizing such hydrogels. These flexible wearable mechanosensors can monitor diverse body movements such as joint bending, walking, running, and stair climbing. This work is anticipated to offer promising soft materials for efficient mechanical-to-electrical signal conversion and provides new insights into the development of various wearable mechanosensors.

OneTip: A Soft Tactile Interface for 6-D Fingertip Pose Acquisition in Human-Computer Interaction

Advances in display technology have created the need for more efficient and natural multi-degree-of-freedom interaction devices. The movement of a single fingertip has six degrees of freedom (DOFs), but traditional rigid touchscreens usually sense only 2-D information. This article proposes a new deformable tactile interface, OneTip, for single-fingertip human-computer interaction with 6 DOFs. It is manufactured based on the principle of vision-based tactile sensing using virtual stereoscopic cameras, and its size is about twice that of a thumb. The contact surface of OneTip has a specially designed structure and material to mimic the sensitivity and softness of human skin. Also, OneTip employs a new sensing method to address the problem of soft fingertip pose estimation (measuring relative change only) with incipient slip effects. Experiments show that OneTip has good 6-D pose estimation accuracy, with root mean square errors (RMSE) of translation and rotation not exceeding 0.1mm and 2.6°, respectively, within the linear interval (x and y: −1.2 to 1.2mm; z: 0 to 3mm; yaw: −15 to 15deg; pitch and roll: −40 to 40deg). Experiments were also conducted to explore the application of OneTip in typical virtual manipulation tasks and the possibility of combining it with other interaction devices.

Plant-based marbled salami analogs: Emulsion-loaded microgels embedded within protein-polysaccharide hydrogel matrices

The inherent molecular differences between plant and animal proteins make it challenging to accurately simulate the optical and mechanical properties of real meat products using plant-derived ingredients. Soft matter physics approaches are therefore being employed to direct the assembly of plant proteins, polysaccharides, and lipids into meat-like structures. The main focus of the current study was to use soft matter physics approaches to create plant-based analogs of marbled meat products, such as salami, chorizo, or pepperoni. These products have whitish fatty regions embedded within reddish/brown lean regions. In this study, we mimicked the fatty regions in salami using emulsion-loaded alginate beads and the lean regions using composite hydrogels assembled from potato protein and gellan gum. Initially, the textural attributes of the plant-based lean regions were optimized by varying potato protein type (low or high isoelectric point) and concentration. As expected, the mechanical strength of the lean region analogs increased with increasing protein content and depended on protein type. Introducing alginate beads into the salami analogs had little impact on their textural attributes when measured under compression conditions but decreased their stiffness and fracture stress when measured under tensile conditions. In particular, introducing either small or large beads reduced the stiffness and breaking stress of the salami analogs, which was attributed to the introduction of weak points in the composite hydrogel. Finally, we showed that the appearance and textural attributes of real salami could be mimicked in plant-based salami by optimizing its composition and structure. This research provides valuable insights into methods of better simulating the properties of marbled meat products, like sausages and cold-cut meat products, thereby creating a more sustainable food supply.

Room temperature self-healing and high gas barrier properties of elastomer composites incorporated with liquid metal

Flexible electronic devices require stretchable packaging materials that provide a hermetic seal. However, conventional soft materials often exhibit strong gas permeability, making it difficult to achieve stable operation, which requires films with high deformability, self-healing capability, and gas barrier functionality. In this study, a layer by layer (LBL) method was employed to uniformly coat a controllable thickness of liquid metal (LM) onto a designed and synthesized self-healing thermoplastic polyurethane (TPU) film, successfully developing a stretchable gas barrier film (TPU/LM) with high gas barrier properties. The designed polyurethane film significantly enhanced the adhesion of the liquid metal, effectively preventing leakage. The experimental results show that the water vapor transmission rate (WVTR) of the TPU/LM composite film with a thickness of 40 μm is 4.04g/(m2·day). Compared to the film without LM, the gas barrier performance has been improved by approximately 16 times. Additionally, there is a significant enhancement in nitrogen (N2) barrier, with a permeation rate reaching 4.0*10−17 cm3 cm/(cm2·s·Pa), effectively blocking the N2 permeation. This demonstrates the universality of the TPU/LM in gas barrier applications. Furthermore, the TPU/LM film also demonstrated excellent electromagnetic shielding effectiveness. The self-healing capability of the stretchable gas barrier film allows it to recover its initial gas barrier performance after mechanical damage. Humidity-sensitive resistors encapsulated with TPU/LM exhibited stable operation in both air and 90 % humidity environments, confirming the superior barrier properties of the TPU/LM. Generally, the developed TPU/LM is suitable for packaging applications in the next generation of flexible electronic devices.

Chemical Auxiliary for Photocatalytic Active Colloids.

Active colloids with the ability to self-propel and collectively organize are emerging as indispensable elements in microrobotics and soft matter physics. For chemically powered colloids, their activity is often induced by gradients of chemical species in the particle's vicinity. The direct manipulation of these gradients, however, presents a considerable challenge, thereby limiting the extent to which active colloids can be controlled. Here, we introduce a series of rationally designed molecules, denoted as chemical auxiliary (CA), that intervene with specific chemical gradients and thus unveil new capabilities for regulating the behaviors of photocatalytic active colloids. We show that CA can alter the diffusiophoretic and osmotic interactions between active colloids and their subsequent self-organization. Also, CA can tune the self-propulsion of active particles, enabling a record high propulsion speed of over 100 μm/s and endowing high salt tolerance. Furthermore, CA is instrumental in establishing dynamic, competing gradients around active particles, which signifies an in situ, noninvasive, and reversible strategy for reconfiguring between modes of colloidal activity.

Parametric Investigation of Rotary Type Magnetorheological Finishing Operation by Batch Gradient Descent Algorithm

Background: The consistency of the magnetorheological process insisted that the Inconel® 718 material should be furnished. This process involves every material from the categories of soft and hard materials. Aim: In this study, a cylindrical ferromagnetic work-part was finished using the magnetorheological finishing method. Objective: The strength of the magnetic flux controls the density and forces in processes that are assisted by magnetic fields. The mechanism was studied parametrically in this research work using response surface methodology Methods: Optimal process parameters were determined using response surface methodology to accurately execute the finishing procedure. Each parameter's percentage consumption to the process's finishing output was also estimated. The finishing of an industrial extrusion punch was carried out using the optimum parameters obtained from the parametric analysis. Results: The RSM optimisation of process parameters is validated using the batch gradient descent (BGD) algorithm which is the best fit and innovation algorithm for these types of optimization solutions. The mathematical model that BGD provides confirms the RSM mathematical model. Conclusion: The optimized parameters are useful in controlling the capability of the MR finishing process in various industrial applications.

Peculiarities of Hematite Reduction Using Waste Activated Sludge (WAS) Carbonization Products

In the present study, XRD, SEM/EDS, Raman, EMR/EPR spectroscopy, and vibrating sample magnetometry (VSM) were used to analyze the reduction of hematite by the carbonization products of waste activated sludge (WAS) at 500–1000 °C. The reduction process includes the following steps: α-Fe2O3 → Fe2O3 + Fe3O4 (Ttr~500 °C) → Fe3O4 (Ttr~600–700 °C) → FeO → Feamorph. (Ttr~1000 °C). The prevalence of certain phase compositions at different hematite reduction temperatures makes it possible to predict the areas viable for the application of reduced oxides: adsorbents (after Ttr~500 °C) → soft ferromagnetic materials (after Ttr~600–700 °C) → electrically engineered amorphous iron (after Ttr~1000 °C).

Understanding the effects of mineralization and structure on the mechanical properties of tendon-bone insertion using mesoscale computational modeling

Tendon-bone fibrocartilaginous insertion, or enthesis, is a specialized interfacial region that connects tendon and bone, effectively transferring forces while minimizing stress concentrations. Previous studies have shown that insertion features gradient mineralization and branching fiber structure, which are believed to play critical roles in its excellent function. However, the specific structure-function relationship, particularly the effects of mineralization and structure at the mesoscale fiber level on the properties and function of insertion, remains poorly understood. In this study, we develop mesoscale computational models of the distinct fiber organization at tendon-bone insertions, capturing the branching network from tendon to interface fibers and the different mineralization scales. We specifically analyze three key descriptors: the mineralization scale of interface fibers, the mean, and relative standard deviation of the local branching angles of interface fibers. Tensile test simulations on insertion models with varying mineralization scales of interface fibers and structures are performed to mimic the primary loading condition applied to the insertion. We measure and analyze five representative mechanical properties: Young's modulus, strength, toughness, resilience, and failure strain. Our results reveal that mechanical properties are significantly influenced by the three key descriptors, with tradeoffs observed between mutually exclusive properties. For instance, strength and resilience plateau beyond a certain mineralization scale, while failure strain and Young's modulus exhibit monotonic decreasing and increasing trends, respectively. Consequently, there exists an optimal mineralization scale for toughness due to these tradeoffs. By analyzing the mesoscale deformation and failure mechanisms from simulation trajectories, we identify three fracture regimes closely related to the trends in mechanical properties, supporting the observed tradeoffs. Additionally, we examine in detail the effects of the mean and relative standard deviation of local branching angles on mechanical properties and deformation mechanisms. Overall, our study enhances the fundamental understanding of the composition-structure-function relationships at the tendon-bone insertion, complementing recent experimental studies. The mechanical insights from our work have the potential to guide the future biomimetic design of fibrillar adhesives and interfaces for joining soft and hard materials.

Photonic defect modes in cholesteric liquid crystal resonators with embedded isotropic layers

Photonic defect modes are explored as a viable alternative to standard photonic band edge modes in photonic crystal applications, especially due to their typically high Q-factors and local density of states. For example, they can be used in nonlinearity enhancement, lasing, and cavity quantum electrodynamics. However, they are strongly dependent on any structural change and need to be well-controlled to ensure the desired resonance frequency. Here, we present a study of the photonic defect modes that appear in a structure where a layer of isotropic material is embedded between two layers of cholesteric liquid crystal (CLC), using full electrodynamics numerical simulations. We present typical transmission spectra and electric field profiles of selected defect modes and then analyze the influence of geometrical and material parameters on the eigenfrequencies and Q-factors of the modes within and around the photonic bandgap, including refractive indices and thicknesses of isotropic and liquid crystal layers, and different anchoring orientations at the boundaries of the isotropic defect layer. Additionally, a connection of such defect modes to previously extensively analyzed twist defect modes is given. Eigenmodes in asymmetric resonators are also presented, where CLC layers surrounding the intermediate isotropic layer are not equally thick, enabling biasing of specific directional light emission. More generally, this work aims to contribute to the understanding and design capability in topological soft matter photonics where defect mode lasing could be realized in CLC geometries with different singular and solitonic topological defect structures.

Responsive Soft Interface Liquid Crystal Microfluidics

AbstractThe multifunctional responsive interfaces of liquid crystal (LC) and water are employed in fundamental research (colloidal assembly) and promising applications (sensing, release, and material synthesis). The stagnant LC systems, however, limit their use in continuous, automated applications. A microfluidic platform is reported where stable LC flow is maintained between aqueous interfaces. The LC‐water soft interface is defined by the preferential wetting of the two phases at the chemically heterogeneous microchannel interfaces. It is shown that the LC‐water interfaces are stable up to significant pressure differences across the interfaces and maintain responsive characteristics. The stability is in a range to cover the perpendicular and flow‐aligned regimes at low and high flow velocities, respectively, in co‐current or counter‐current flow configurations. The LC configuration at the vicinity of the aqueous interfaces is influenced by the shear induced by the bulk LC flow and by the contacting aqueous phases allowing modulation of the LC strain at the responsive interfaces. The simplicity of the construction and operation of the soft‐interface LC flow platform shows promise and meets the fundamental requirements for their integration into next‐generation autonomous platforms.

Unveiling the interfacial liquid in electrochemical reactions

Adapting novel experimental techniques to address key knowledge gaps about the structure and properties of the interfacial liquid (IL) will enhance our understanding of its influence on electrochemical reactions, particularly in mediating species transport, charge transfer, and intermediate stability.

Biomimetic Soft Robotic Jellyfish for Lentic Ecosystem Monitoring

Environmental monitoring of lentic ecosystems is well suited for swarm robotics applications since they can operate autonomously and cover large regions. For such a task, a locomotion mechanism is necessary for traversal. Due to the challenging nature of underwater environments, researchers often draw inspiration from nature to improve robot mechanical performance. A box jellyfish in a good inspiration due to their efficient jet propulsion. Soft and smart materials are helpful in mimicking their propulsion because they can perform flexible and complex movement. Shape memory alloy (SMA) springs have been used for this purpose, but their slow actuation rate is a well-known disadvantage. This project aims to improve cycle rate and thus swim speed by implementing a bistable spring configuration into a soft robotic jellyfish. The bistable mechanism stores energy slowly in the expansion of the elastic silicone bell, then releases it suddenly in a contraction which propels the robot forwards with a higher force than would be possible with direct SMA actuation. Additionally, the antagonistic arrangement of SMA springs reset each other and produce the same outward expansion on both up and down stroke, improving cycles speeds by removing the need for a dedicated reset stroke which is typically required before using the springs again. Also, increasing the number of spring pairs does not interfere with the actuation, meaning cycle rates can be further improved by cycling which pair of springs is active. The proof-of-concept device operates at a frequency of 0.4 Hz, and produces enough thrust while tethered to swim through a tank. Future work involves performing fluid visualization tests to validate a simple mathematical model of flow through the bell, as well as optimize the design, integrate onboard environment sensors and implement autonomy to allow operation in a larger swarm.

Engineered Janus hydrogels: biomimetic surface engineering and biomedical applications.

Hydrogel bioadhesives, when applied to dysfunctional tissues substituting the epidermis or endothelium, exhibit compelling characteristics that enable revolutionary diagnostic and therapeutic procedures. Despite their demonstrated efficacy, these hydrogels as soft implants are still limited by improper symmetric surface functions, leading to postoperative complications and disorders. Janus hydrogel bioadhesives with unique asymmetric surface designs have thus been proposed as a reliable and biocompatible hydrogel interface, mimicking the structural characteristics of natural biological barriers. In this comprehensive review, we provide guidelines for the rational design of Janus hydrogel bioadhesives, covering methods for hydrogel surface chemistry and microstructure engineering. The engineering of Janus hydrogels is highlighted, specifically in tuning the basal surface to facilitate instant and robust hydrogel-tissue integration and modulating the apical surface as the anti-adhesion, anti-fouling, and anti-wear barrier. These asymmetric designs hold great potential in clinical translation, supporting applications including hemostasis/tissue sealing, chronic wound management, and regenerative medicine. By shedding light on the potential of Janus hydrogels as bioactive interfaces, this review paper aims to inspire further research and overcome current obstacles for advancing soft matter in next-generation healthcare.

Smart heat management flexible cellulose films with enhanced thermal conductivity via assembling graphene and boron nitride nanosheets

Smart materials with high thermal conductivity are expected to have greatly application potential in thermal management for future electronic equipment. However, actual applications often require multifunctional properties of materials, such as high thermal conductivity (TC), good mechanical properties, and suitable electrical insulation performance. It is still a challenge to obtain such polymer composites with good comprehensive properties. Herein, the rational assembly of two-dimensional (2D) nanofillers of boron nitride nanosheets (BNNS) and graphene nanosheets (GNs) in nanofibrillated cellulose matrix is reported. The film shows 53.76 W m−1 K−1 of TC and 87.88 MPa of tensile strength. Meanwhile, the flexible film has the ability of response deformation by sensing the environmental temperature, which is promising for soft materials with excellent heat dissipation.

Manufacture process and cabling optimization of Bi2212 CICC

The Bi2212 cable-in-conduit conductor (CICC) is a composite soft material and is sensitive to stress-strain and brittle breakage. The cabling tensions are critical parameters for the CICCs and have undergone trial production many times to achieve effective cable control. Unreasonable tension will cause circumferential and axial motion, resulting in deflection bending, rotation fluctuations, and wire slip. This study investigated the manufacturing process of the Bi2212 CICC, optimizing the cable twisting process and reducing manufacturing consumption and damage. Additionally, optimized tensions of the Bi2212 CICCs during the cabling process, focusing on pay-off tension, rotation speeds, and traction tensions were presented. Finally, the results are tested and verified in the factory to examine the wire jumpers, serpentine bending, and pitch fluctuations. This research provides useful references for future cable fabrication of the HTS CICCs.