Search

Wearable flexible sensors based on conductive hydrogels have received extensive attention in the fields of electronic skin and smart monitoring. However, conductive hydrogels contain a large amount of water, which greatly affects their performances in harsh environments. It is therefore necessary to prepare hydrogel sensors that are stable at low temperatures. Herein, metal ions (MgCl 2 ) and ethylene glycol (EG) were combined with polyvinyl alcohol (PVA) to obtain a conductive PVA/EG hydrogel with tensile strength and elongation at break of 1.1 MPa and 442.3 %, respectively, which could withstand >6000-fold its own weight. The binary solvent system composed of water and EG contributed to the excellent anti-freezing properties and long-term storage (>1 week), flexibility, and stability of the hydrogel even at -20 °C. The wearable PVA/EG hydrogel as a flexible sensor possessed desirable sensing performances with a competitive GF value of 0.725 and fatigue resistance (50 cycles) when used to monitor various human motions and physiological signals. Overall, this hydrogel sensor shows strong potential for application in the fields of human motion monitoring, written information sensing, and information encryption and transmission., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2023 Elsevier B.V. All rights reserved.)

A fluorescent and colorimetric poly (acrylamide)-based copolymer probe P(AAm-co-RBNCH) has been designed via free radical polymerization of a commercial acrylamide monomer with a rhodamine-functionalized monomer RBNCH. Metal ion selectivity of RBNCH was investigated by fluorescence and colorimetric spectrophotometry. Upon addition of Fe3+, a visual color change from colorless to red and a large fluorescence enhancement were observed for the ring-opening of the rhodamine spirolactam mechanism. The monomer gives a sensitive method for quantitatively detecting Fe3+ in the linear range of 100–200 μM, with a limit of detection as low as 27 nM and exhibiting high selectivity for Fe3+ over 12 other metal ions. The hydrogel sensor was characterized by FTIR, and the effects of RBNCH amount on gel content and swelling properties were explored. According to the recipe of 1.0 mol% RBNCH to the total monomers, the fabricated hydrogel sensor displayed a good swelling property and reversibility performance and has potential for application in the imaging of Fe3+ level in industrial wastewater. [ABSTRACT FROM AUTHOR]

Stimuli-responsive color-changing and shape-changing hydrogels are promising intelligent materials for visual detections and bio-inspired actuations, respectively. However, it is still an early stage to integrate the color-changing performance and shape-changing performance together to provide bi-functional synergistic biomimetic devices, which are difficult to design but will greatly expand further applications of intelligent hydrogels. Herein, we present an anisotropic bi-layer hydrogel by combining a pH-responsive rhodamine-B (RhB)-functionalized fluorescent hydrogel layer and a photothermal-responsive shape-changing melanin-added poly (N-isopropylacrylamide) (PNIPAM) hydrogel layer with fluorescent color-changing and shape-changing bi-functional synergy. This bi-layer hydrogel can obtain fast and complex actuations under irradiation with 808 nm near-infrared (NIR) light due to both the melanin-composited PNIPAM hydrogel with high efficiency of photothermal conversion and the anisotropic structure of this bi-hydrogel. Furthermore, the RhB-functionalized fluorescent hydrogel layer can provide rapid pH-responsive fluorescent color change, which can be integrated with NIR-responsive shape change to achieve bi-functional synergy. As a result, this bi-layer hydrogel can be designed using various biomimetic devices, which can show the actuating process in the dark for real-time tracking and even mimetic starfish to synchronously change both the color and shape. This work provides a new bi-layer hydrogel biomimetic actuator with color-changing and shape-changing bi-functional synergy, which will inspire new strategies for other intelligent composite materials and high-level biomimetic devices. [ABSTRACT FROM AUTHOR]

The human skin, an important sensory organ, responds sensitively to external stimuli under various harsh conditions. However, the simultaneous achievement of mechanical/thermal sensitivity and extreme environmental tolerance remains an enormous challenge for skin‐like hydrogel‐based sensors. In this study, a novel skin‐inspired hydrogel–elastomer hybrid with a sandwich structure and strong interfacial bonding for mechanical–thermal multimode sensing applications is developed. An inner‐layered ionic hydrogel with a semi‐interpenetrating network is prepared using sodium carboxymethyl cellulose (CMC) as a nanofiller, lithium chloride (LiCl) as an ionic transport conductor, and polyacrylamide (PAM) as a polymer matrix. The outer‐layered polydimethylsiloxane (PDMS) elastomers fully encapsulating the hydrogel endow the hybrids with improved mechanical properties, intrinsic waterproofness, and long‐term water retention (>98%). The silane modification of the hydrogels and elastomers imparts the hybrids with enhanced interfacial bonding strength and integrity. The hybrids exhibit a high transmittance (~91.2%), fatigue resistance, and biocompatibility. The multifunctional sensors assembled from the hybrids realize real‐time temperature (temperature coefficient of resistance, approximately −1.1% °C−1) responsiveness, wide‐range strain sensing capability (gauge factor, ~3.8) over a wide temperature range (from −20°C to 60°C), and underwater information transmission. Notably, the dual‐parameter sensor can recognize the superimposed signals of temperature and strain. The designed prototype sensor arrays can detect the magnitude and spatial distribution of forces and temperatures. The comprehensive performance of the sensor prepared via a facile method is superior to that of most similar sensors previously reported. Finally, this study develops a new material platform for monitoring human health in extreme environments. [ABSTRACT FROM AUTHOR]

[Display omitted] The flexible and self-healing supercapacitors (SCs) are considered to be promising smart energy storage devices. Nevertheless, the SCs integrated with flexibility, lightweight, pattern editability, self-healing capabilities and desirable electrochemical properties remain a challenge. Herein, an all-in-one self-healing SC fabricated with the free-standing hybrid film (TCMP) composed of the 2,2,6,6-tetramethylpiperidin-1-yloxy-oxidized cellulose nanofibers (TOCNs) carried carbon nanotubes (CNTs), manganese dioxide (MnO 2) and polyaniline (PANI) as the electrode, polyvinyl alcohol/sulfuric acid (PVA/H 2 SO 4) gel as the electrolyte and dynamically cross-linked cellulose nanofibers/PVA/sodium tetraborate decahydrate (CNF/PB) hydrogel as the self-healing electrode matrix is developed. The TCMP film electrodes are fabricated through a facile in-situ polymerization of MnO 2 and PANI in TOCNs-dispersed CNTs composite networks, exhibiting lightweight, high electrical conductivity, flexibility, pattern editability and excellent electrochemical properties. Benefited from the hierarchically porous structure and high mechanical properties of TOCNs, excellent electrical conductivity of CNTs and the desirable synergistic effect of pseudocapacitance induced by MnO 2 and PANI, the assembled SC with an interdigital structure demonstrated a high areal capacitance of 1108 mF cm−2 at 2 mA cm−2, large areal energy density of 153.7 μWh cm−2 at 1101.7 μW cm−2. A satisfactory bending cycle performance (capacitance retention up to 95 % after 200 bending deformations) and self-healing characteristics (∼90 % capacitance retention after 10 cut/repair cycles) are demonstrated for the TCMP-based symmetric SC, delivering a feasible strategy for electrochemical energy storage devices with excellent performance, designable patterns and desirable safe lifespan. [ABSTRACT FROM AUTHOR]

Inspired by creatures, abundant stimulus-responsive hydrogel actuators with diverse functionalities have been manufactured for applications in soft robotics. However, constructing a shape memory and self-sensing bilayer hydrogel actuator with high mechanical strength and strong interfacial bonding still remains a challenge. Herein, a novel bilayer hydrogel with a stimulus-responsive TEMPO-oxidized cellulose nanofibers/poly(N-isopropylacrylamide) (TOCN/PNIPAM) layer and a non-responsive TOCN/polyacrylamide (TOCN/PAM) layer is proposed as a thermosensitive actuator. TOCNs as a nano-reinforced phase provide a high mechanical strength and endow the hydrogel actuator with a strong interfacial bonding. Due to the incorporation of TOCNs, the TOCN/PNIPAM hydrogel exhibits a high compressive strength (~89.2 kPa), elongation at break (~170.7 %) and tensile strength (~24.0 kPa). The prepared PNIPAM/TOCN/PAM hydrogel actuator performs the roles of an encapsulation, jack, temperature-controlled fluid valve and temperature-control manipulator. The incorporation of Fe3+ further endows the bilayer hydrogel actuator with a synergistic performance of shape memory and temperature-driven, which can be used as a temperature-responsive switch to detect ambient temperature. The PNIPAM/TOCN/PAM-Fe3+ conductive hydrogel can be assembled into a flexible sensor and generate sensing signals when driven by temperature changes to achieve real-time feedback. This research may lead to new insights into the design and manufacturing of intelligent flexible soft robots. [Display omitted] [ABSTRACT FROM AUTHOR]

• A green and common method was proposed to prepare biomimetic actuators. • The PNPB actuator showed excellent multi-stimulus response and synergistic effect. • Anisotropic natural bamboo endowed the PNPB actuator programmable performance. • The PNPB actuator had application potential in complex environment. Hydrogel actuators with controllable deformation and excellent biocompatibility are widely used in soft robot, valve, drug delivery and lenses. However, the stimulation response performance of existing hydrogel actuators mostly focuses on a single active layer, which greatly affects its driving performance and service life. In this work, we integrate temperature-responsive hydrogel (Poly (N-isopropyl acrylamide), PNIPAM) and pH-responsive hydrogel (polyacrylic acid, PAAc) into one system to fabricate a dual active layer composite hydrogel actuator with high performance. Based on the PAAc hydrogels achieving contract or expand at different pH values, the obtained actuator exhibits admirable bidirectional bending characteristics. In addition, the anisotropic bamboo sheet endows the hydrogel actuator with programmable 3 D complex deformation. Benefitting from the synergy and different responsiveness between the two active layers, the hydrogel actuator not only has multiple response performance, but also greatly improves its deformation degree and response speed. More importantly, these promising properties of the actuator have broad application prospects in the development of pattern design and intelligent switch. This work proposes a promising strategy for the structural design of hydrogel actuators with excellent performance, and encourages more exploration of the application range of the actuator. [ABSTRACT FROM AUTHOR]

• The morph-genetic method was innovatively used to fabricate the ABH actuator. • The ABH actuator exhibits promising comprehensive performance. • The assembled biomimetic actuators show excellent synergistic performance. • The biomimetic actuator shows potential for a variety of applications. Stimuli-responsive hydrogels are most promising for the fabrication of autonomous bio-mimetic soft actuators. However, their weak actuation forces and isotropic volume change hinder their practical utilization as versatile actuators, owing to their fragility. Herein, we used the morph-genetic method to fabricate anisotropic bamboo/poly(N-isopropylacrylamide) hydrogel (ABH) complex for use as soft actuator. First of all, the bamboo fiber structure provides an anisotropic framework for the ABH actuator to achieve precise deformational programmability. Secondly, benefiting from the ultra-high directional strength (110 MPa) of bamboo, ABH actuator exhibits sufficiently robust mechanical property, which generates a powerful actuating force. Lastly, owing to the regulation of bamboo sheet and PNIPAM hydrogel, the ABH actuator not only achieves ultra-fast response speed (825°/s of the bending speed), but also has excellent synergetic performance. We demonstrate several bio-mimetic actuating devices based on ABH actuator, inspired by the intricate motions of natural organisms, to highlight how the specific materials properties and their synergy can be systematically exploited for the rational design of soft actuators. Henceforth, it is anticipated that the development of hydrogel actuators could continue to benefit from the use of various naturally-anisotropic materials, such as shape-memory polymers or liquid crystals, for the preparation of further advanced hydrogel actuators by the morph-genetic method. [ABSTRACT FROM AUTHOR]

• PPy-coated P(NIPAM-ABP) electrospun nanofiber can provide high strength. • PPy-coating by in situ polymerization can provide high light-responsive. • The actuator owns ultrafast deformation and rapid recovery. • The actuator can realize various 3D programmable complex deformations. • We have explored new biomimetic devices based on the advantages of the actuator. Intelligent hydrogels are promising for biomimetic actuators, but acquiring actuations with both high speed and powerful force is still extremely difficult. Herein, a new robust polypyrrole (PPy)-coated copoly(isopropylacrylamide-4-benzoylphenyl acrylate) [P(NIPAM-ABP)] electrospun light-responsive hydrogel is explored. The (PPy)-coated P(NIPAM-ABP) hydrogel can be obtained via in-situ polymerization of pyrroles on the nanofiber-oriented electrospun P(NIPAM-ABP) hydrogel. Compared with original P(NIPAM-ABP) hydrogel, this PPy-coated P(NIPAM-ABP) hydrogel can integrate highly-enhanced mechanical strength (from 1.21 to 5.12 MPa of tensile strength) and ultrahigh-efficiency of photothermal conversion together. In addition, the orientation of P(NIPAM-ABP) nanofibers can still maintain well for programmable complex deformations. Consequently, the as-prepared robust bi-hydrogel actuator with ultrafast and complex deformations has been achieved, through bonding the PPy-P(NIPAM-ABP) hydrogel membrane with a polyethylene glycol diacrylate-cellulose nanofiber (PEGDA-CNF) composite hydrogel membrane via interfacial ultraviolet (UV) polymerization of PEGDA monomers. Several light-responsive biomimetic actuating devices have been achieved, which owning powerful force (can grab up 100 times of self-weight), rapid speed (1285.71°/s of folding) or precisely programmable complex deformations. Furthermore, two biomimetic devices with synergistic functions of the three advantages above have been explored, which can mimic the child's sit-up and the starfish's continuous crawling movement respectively. This work provides a robust remotely-controlled light-responsive hydrogel actuator with powerful force, ultrafast speed and programmable complex actuations, which will inspire the design and fabrication of novel soft biomimetic actuating materials and systems. [ABSTRACT FROM AUTHOR]

Near-infrared light-responsive hydrogel actuator with complex deformations and remote precise control is fabricated from the natural bamboo. The resulting biomimetic bamboo/PNIPAM hydrogel actuator can be precisely designed to perform a variety of simulations. [Display omitted] • Biomimetic actuators based on anisotropic natural bamboo were prepared. • Nigrosine was first used to fabricate light-responsive hydrogel actuator. • The actuator exhibits outstanding programmability and remote-control performance. • The actuator can move freely on the water surface based on Marangoni effect. Near-infrared light-responsive hydrogels are one of the most important soft biomimetic actuators owing to their accuracy, remote control performance, and permeability. However, the complex deformations and materials of hydrogel actuators are still a serious challenge. Herein, we have developed a novel composite hydrogel actuator by combining natural bamboo sheet and nigrosine/poly(N-isopropylacrylamide) (PNIPAM) composite hydrogel. The high-efficient photothermal conversion of the nigrosine/PNIPAM composite hydrogel sheet generates light-responsive actuation that is remotely controllable. Furthermore, the bamboo sheet with fiber-oriented structure can be cut at different angles, which facilitates programmable 3D complex deformations in the actuator. Accordingly, we have designed a series of biomimetic actuating devices, including simulations of butterfly antenna, Dendrobium , smart switch, and even a multi-step deformational biomimetic claw. In addition, we also explored a biomimetic insect with precisely-controlled fast movements on the water surface based on Marangoni effect. This work provides a simple but general strategy for fabricating biomimetic actuators and will inspire new designs for intelligent soft actuators. [ABSTRACT FROM AUTHOR]

[Display omitted] • The actuator can achieve synergistic movement of deformation and transportation. • Added Fe 3 O 4 NPs provide both magnetism and high-efficient photothermal conversion. • The hydrogel actuator owns high tensile-strength of 4.59 MPa via electrospinning. • The actuator can provide ultrafast deformational speed of 178°/s. • We have explored new bio-inspired systems with two/multi-step synergic actuation. As a soft/wet intelligent material, hydrogel actuators with multiple stimuli-responsiveness have been widely developed. However, it is still greatly difficult for them to integrate bi/multiple responsiveness together for bio-mimetic synergistic actuation. Here, we have explored a high-strength anisotropic bi-layer hydrogel actuator with P(NIPAM-ABP) layer and Fe 3 O 4 /PAN layer via electrospinning technique, which can provide programmable bi-functional synergistic movement. The Fe 3 O 4 /PAN layer can provide magnetic responsive navigation for long-range transportation on account of the magnetism of the Fe 3 O 4 nanoparticles. Furthermore, the ultrahigh photothermal conversion efficiency of the Fe 3 O 4 nanoparticles in the Fe 3 O 4 /PAN layer, can endow the P(NIPAM-ABP) layer with fast remotely-controlled photothermal-responsive deformation. Most importantly, this hydrogel actuator can achieve complex higher-level programmable movements than before based on the synergy of remotely-controlled deformation and the long-range transportation, which can be utilized to design various novel bio-mimetic soft-robots. Last but not least, the introduction of the electrospinning, not only can achieve high strength (4.59 MPa of tensile strength) of this bi-layer hydrogel, but also can provide both ultrafast (178°/s) and programmable complex photothermal-responsiveness, owing to the ultrahigh specific surface area (ultra-thin and porous structure) and excellent orientation of the thermal-responsive P(NIPAM-ABP) nanofibers respectively. This work will provide a general method via electrospinning for anisotropic hydrogel actuator with bi/multiple-functional synergy and will provide a new strategy for smart actuators and other bio-mimetic intelligent materials/systems. [ABSTRACT FROM AUTHOR]