Showing papers on "Self-healing hydrogels published in 2018"

Mussel-Inspired Adhesive and Conductive Hydrogel with Long-Lasting Moisture and Extreme Temperature Tolerance

Abstract: Conductive hydrogels are a promising class of materials to design bioelectronics for new technological interfaces with human body, which are required to work for a long-term or under extreme environment. Traditional hydrogels are limited in short-term usage under room temperature, as it is difficult to retain water under cold or hot environment. Inspired by the antifreezing/antiheating behaviors from nature, and based on mussel chemistry, an adhesive and conductive hydrogel is developed with long-lasting moisture lock-in capability and extreme temperature tolerance, which is formed in a binary-solvent system composed of water and glycerol. Polydopamine (PDA)-decorated carbon nanotubes (CNTs) are incorporated into the hydrogel, which assign conductivity to the hydrogel and serve as nanoreinforcements to enhance the mechanical properties of the hydrogel. The catechol groups on PDA and viscous glycerol endow the hydrogel with high tissue adhesiveness. Particularly, the hydrogel is thermal tolerant to maintain all the properties under extreme wide tempreature spectrum (−20 or 60 °C) or stored for a long term. In summary, this mussel-inspired hydrogel is a promising material for self-adhesive bioelectronics to detect biosignals in cold or hot environments, and also as a dressing to protect skin from injuries related to frostbites or burns.

Mussel-Inspired Cellulose Nanocomposite Tough Hydrogels with Synergistic Self-Healing, Adhesive, and Strain-Sensitive Properties

Abstract: The remarkable progress in efforts to prepare conductive self-healing hydrogels mimicking human skin’s functions has been witnessed in recent years. However, it remains a great challenge to develop an integrated conductive gel combining excellent self-healing and mechanical properties, which is derived from their inherent compromise between the dynamic cross-links for healing and steady cross-links for mechanical strength. In this work, we design a tough, self-healing, and self-adhesive ionic gel by constructing synergistic multiple coordination bonds among tannic acid-coated cellulose nanocrystals (TA@CNCs), poly(acrylic acid) chains, and metal ions in a covalent polymer network. The incorporated TA@CNC acts as a dynamic connected bridge in the hierarchically porous network mediated by multiple coordination bonds, endowing the ionic gels the superior mechanical performance. Reversible nature of dynamic coordination interactions leads to excellent recovery property as well as reliable mechanical and elect...

MXenes stretch hydrogel sensor performance to new limits

Abstract: The development of wearable electronics, point-of-care testing, and soft robotics requires strain sensors that are highly sensitive, stretchable, capable of adhering conformably to arbitrary and complex surfaces, and preferably self-healable. Conductive hydrogels hold great promise as sensing materials for these applications. However, their sensitivities are generally low, and they suffer from signal hysteresis and fluctuation due to their viscoelastic property, which can compromise their sensing performance. We demonstrate that hydrogel composites incorporating MXene (Ti3C2T x ) outperform all reported hydrogels for strain sensors. The obtained composite hydrogel [MXene-based hydrogel (M-hydrogel)] exhibits outstanding tensile strain sensitivity with a gauge factor (GF) of 25, which is 10 times higher than that of pristine hydrogel. Furthermore, the M-hydrogel exhibits remarkable stretchability of more than 3400%, an instantaneous self-healing ability, excellent conformability, and adhesiveness to various surfaces, including human skin. The M-hydrogel composite exhibits much higher sensitivity under compressive strains (GF of 80) than under tensile strains. We exploit this asymmetrical strain sensitivity coupled with viscous deformation (self-recoverable residual deformation) to add new dimensions to the sensing capability of hydrogels. Consequently, both the direction and speed of motions on the hydrogel surface can be detected conveniently. Based on this effect, M-hydrogel demonstrates superior sensing performance in advanced sensing applications. Thus, the traditionally disadvantageous viscoelastic property of hydrogels can be transformed into an advantage for sensing, which reveals prospects for hydrogel sensors.

Multifunctional Stimuli-Responsive Hydrogels with Self-Healing, High Conductivity, and Rapid Recovery through Host–Guest Interactions

Abstract: Self-healing hydrogels with multifunctionality as a type of fascinating material show potential application in various fields, such as biomedicine, tissue engineering, and wearable electronic devices. However, to combine the properties of autonomous self-healing property, high conductivity, excellent mechanical properties, and stimuli-responsive properties for hydrogel is still a great challenge. Herein, we present self-healing conductive hydrogels based on β-cyclodextrin (β-CD), N-isopropylacrylamide (NIPAM), multiwalled carbon nanotubes (CNT) and nanostructured polypyrrole (PPY). Among them, β-CD served as the host molecule, and NIPAM served as the guest molecule, CNT as the physical cross-linker and conducting substrate, and PPY as the highly conductive component, respectively. The obtained hydrogels exhibit high conductivity, self-healing property, flexible and elastic mechanical property and rapid stimuli-responsive property both to temperature and near-infrared (NIR)-light together. The excellent ch...

Stretchable All-Gel-State Fiber-Shaped Supercapacitors Enabled by Macromolecularly Interconnected 3D Graphene/Nanostructured Conductive Polymer Hydrogels

Abstract: Nanostructured conductive polymer hydrogels (CPHs) have been extensively applied in energy storage owing to their advantageous features, such as excellent electrochemical activity and relatively high electrical conductivity, yet the fabrication of self-standing and flexible electrode-based CPHs is still hampered by their limited mechanical properties. Herein, macromolecularly interconnected 3D graphene/nanostructured CPH is synthesized via self-assembly of CPHs and graphene oxide macrostructures. The 3D hybrid hydrogel shows uniform interconnectivity and enhanced mechanical properties due to the strong macromolecular interaction between the CPHs and graphene, thus greatly reducing aggregation in the fiber-shaping process. A proof-of-concept all-gel-state fibrous supercapacitor based on the 3D polyaniline/graphene hydrogel is fabricated to demonstrate the outstanding flexibility and mouldability, as well as superior electrochemical properties enabled by this 3D hybrid hydrogel design. The proposed device can achieve a large strain (up to ≈40%), and deliver a remarkable volumetric energy density of 8.80 mWh cm-3 (at power density of 30.77 mW cm-3 ), outperforming many fiber-shaped supercapacitors reported previously. The all-hydrogel design opens up opportunities in the fabrication of next-generation wearable and portable electronics.

Highly Stretchable and Tough Hydrogels below Water Freezing Temperature.

Abstract: Hydrogels consist of hydrophilic polymer networks dispersed in water. Many applications of hydrogels rely on their unique combination of solid-like mechanical behavior and water-like transport properties. If the temperature is lowered below 0 °C, however, hydrogels freeze and become rigid, brittle, and non-conductive. Here, a general class of hydrogels that do not freeze at temperatures far below 0 °C, while retaining high stretchability and fracture toughness, is demonstrated. These hydrogels are synthesized by adding a suitable amount of an ionic compound to the hydrogel. The present study focuses on tough polyacrylamide-alginate double network hydrogels equilibrated with aqueous solutions of calcium chloride. The resulting hydrogels can be cooled to temperatures as low as -57 °C without freezing. In this temperature range, the hydrogels can still be stretched more than four times their initial length and have a fracture toughness of 5000 J m-2 . It is anticipated that this new class of hydrogels will prove useful in developing new applications operating under a broad range of environmental and atmospheric conditions.

Stretchable, Transparent, and Self-Patterned Hydrogel-Based Pressure Sensor for Human Motions Detection

Abstract: In this study, a binary networked conductive hydrogel is prepared using acrylamide and polyvinyl alcohol. Based on the obtained hydrogel, an ultrastretchable pressure sensor with biocompatibility and transparency is fabricated cost effectively. The hydrogel exhibits impressive stretchability (>500%) and superior transparency (>90%). Furthermore, the self-patterned microarchitecture on the hydrogel surface is beneficial to achieve high sensitivity (0.05 kPa−1 for 0–3.27 kPa). The hydrogel-based pressure sensor can precisely monitor dynamic pressures (3.33, 5.02, and 6.67 kPa) with frequencydependent behavior. It also shows fast response (150 ms), durable stability (500 dynamic cycles), and negligible current variation (6%). Moreover, the sensor can instantly detect both tiny (phonation, airflowing, and saliva swallowing) and robust (finger and limb motions) physiological activities. This work presents insights into preparing multifunctional hydrogels for mechanosensory electronics.

Nanocellulose-Mediated Electroconductive Self-Healing Hydrogels with High Strength, Plasticity, Viscoelasticity, Stretchability, and Biocompatibility toward Multifunctional Applications.

Abstract: Conducting polymer hydrogels (CPHs) have emerged as a fascinating class of smart soft matters important for various advanced applications. However, achieving the synergistic characteristics of cond...

Highly Stretchable and Biocompatible Strain Sensors Based on Mussel-Inspired Super-Adhesive Self-Healing Hydrogels for Human Motion Monitoring.

Abstract: Integrating multifunctionality such as adhesiveness, stretchability, and self-healing ability on a single hydrogel has been a challenge and is a highly desired development for various applications including electronic skin, wound dressings, and wearable devices. In this study, a novel hydrogel was synthesized by incorporating polydopamine-coated talc (PDA–talc) nanoflakes into a polyacrylamide (PAM) hydrogel inspired by the natural mussel adhesive mechanism. Dopamine molecules were intercalated into talc and oxidized, which enhanced the dispersion of talc and preserved catechol groups in the hydrogel. The resulting dopamine–talc–PAM (DTPAM) hydrogel showed a remarkable stretchability, with over 1000% extension and a recovery rate over 99%. It also displayed strong adhesiveness to various substrates, including human skin, and the adhesion strength surpassed that of commercial double-sided tape and glue sticks, even as the hydrogel dehydrated over time. Moreover, the DTPAM hydrogel could rapidly self-heal a...

Muscle‐Inspired Highly Anisotropic, Strong, Ion‐Conductive Hydrogels

Abstract: Biological tissues generally exhibit excellent anisotropic mechanical properties owing to their well-developed microstructures. Inspired by the aligned structure in muscles, a highly anisotropic, strong, and conductive wood hydrogel is developed by fully utilizing the high-tensile strength of natural wood, and the flexibility and high-water content of hydrogels. The wood hydrogel exhibits a high-tensile strength of 36 MPa along the longitudinal direction due to the strong bonding and cross-linking between the aligned cellulose nanofibers (CNFs) in wood and the polyacrylamide (PAM) polymer. The wood hydrogel is 5 times and 500 times stronger than the bacterial cellulose hydrogels (7.2 MPa) and the unmodified PAM hydrogel (0.072 MPa), respectively, representing one of the strongest hydrogels ever reported. Due to the negatively charged aligned CNF, the wood hydrogel is also an excellent nanofluidic conduit with an ionic conductivity of up to 5 × 10-4 S cm-1 at low concentrations for highly selective ion transport, akin to biological muscle tissue. The work offers a promising strategy to fabricate a wide variety of strong, anisotropic, flexible, and ionically conductive wood-based hydrogels for potential biomaterials and nanofluidic applications.

Rational Fabrication of Anti-Freezing, Non-Drying Tough Organohydrogels by One-Pot Solvent Displacement.

Abstract: Tough hydrogels, polymeric network structures with excellent mechanical properties (such as high stretchability and toughness), are emerging soft materials. Despite their remarkably mechanical features, tough hydrogels exhibit two flaws (freezing around the icing temperatures of water and drying under arid conditions). Inspired by cryoprotectants (CPAs) used in the inhibition of the icing of water in biological samples, a versatile and straightforward method is reported to fabricate extreme anti-freezing, non-drying CPA-based organohydrogels with long-term stability by partially displacing water molecules within the pre-fabricated hydrogels. CPA-based Ca-alginate/polyacrylamide (PAAm) tough hydrogels were successfully fabricated with glycerol, glycol, and sorbitol. The CPA-based organohydrogels remain unfrozen and mechanically flexible even up to -70 °C and are stable under ambient conditions or even vacuum.

Exploring a naturally tailored small molecule for stretchable, self-healing, and adhesive supramolecular polymers

Abstract: Polymeric materials with integrated functionalities are required to match their ever-expanding practical applications, but there is always a trade-off between complex material performances and synthetic simplification. A simple and effective synthesis route is reported to transform a small molecule of biological origin, thioctic acid, into a high-performance supramolecular polymeric material, which combines processability, ultrahigh stretchability, rapid self-healing ability, and reusable adhesivity to surfaces. The proposed one-step preparation process of this material involves the mixing of three commercially available feedstocks at mild temperature without any external solvent and a subsequent cooling process that resulted in a dynamic, high-density, and dry supramolecular polymeric network cross-linked by three different types of dynamic chemical bonds, whose cooperative effects in the network enable high performance of this supramolecular polymeric material.

Optimization of gelatin-alginate composite bioink printability using rheological parameters: a systematic approach.

Abstract: Three-dimensional bioprinting has emerged as a promising technique in tissue engineering applications through the precise deposition of cells and biomaterials in a layer-by-layer fashion. However, the limited availability of hydrogel bioinks is frequently cited as a major issue for the advancement of cell-based extrusion bioprinting technologies. It is well known that highly viscous materials maintain their structure better, but also have decreased cell viability due to the higher forces which are required for extrusion. However, little is known about the effect of the two distinct components of dynamic modulus of viscoelastic materials, storage modulus (G') and loss modulus (G″), on the printability of hydrogel-based bioinks. Additionally, 'printability' has been poorly defined in the literature, mostly consisting of gross qualitative measures which do not allow for direct comparison of bioinks. This study developed a framework for evaluating printability and investigated the effect of dynamic modulus, including storage modulus (G'), loss modulus (G″), and loss tangent (G″/G') on the printing outcome. Gelatin and alginate as model hydrogels were mixed at various concentrations to obtain hydrogel formulations with a wide range of storage and loss moduli. These formulations were then evaluated for the quantitatively defined values of extrudability, extrusion uniformity, and structural integrity. For extrudability, increasing either the loss or storage modulus increased the pressure required to extrude the bioink. A mathematical model relating the G' and G″ to the required extrusion pressure was derived based on the data. A lower loss tangent was correlated with increased structural integrity while a higher loss tangent correlated with increased extrusion uniformity. Gelatin-alginate composite hydrogels with a loss tangent in the range of 0.25-0.45 exhibited an excellent compromise between structural integrity and extrusion uniformity. In addition to the characterization of a common bioink, the methodology introduced in this paper could also be used to evaluate the printability of other bioinks in the future.

Mechanically tunable conductive interpenetrating network hydrogels that mimic the elastic moduli of biological tissue.

Abstract: Conductive and stretchable materials that match the elastic moduli of biological tissue (0.5–500 kPa) are desired for enhanced interfacial and mechanical stability. Compared with inorganic and dry polymeric conductors, hydrogels made with conducting polymers are promising soft electrode materials due to their high water content. Nevertheless, most conducting polymer-based hydrogels sacrifice electronic performance to obtain useful mechanical properties. Here we report a method that overcomes this limitation using two interpenetrating hydrogel networks, one of which is formed by the gelation of the conducting polymer PEDOT:PSS. Due to the connectivity of the PEDOT:PSS network, conductivities up to 23 S m−1 are achieved, a record for stretchable PEDOT:PSS-based hydrogels. Meanwhile, the low concentration of PEDOT:PSS enables orthogonal control over the composite mechanical properties using a secondary polymer network. We demonstrate tunability of the elastic modulus over three biologically relevant orders of magnitude without compromising stretchability ( > 100%) or conductivity ( > 10 S m−1).

Two-Dimensional MXene (Ti3C2)-Integrated Cellulose Hydrogels: Toward Smart Three-Dimensional Network Nanoplatforms Exhibiting Light-Induced Swelling and Bimodal Photothermal/Chemotherapy Anticancer Activity.

Abstract: Two-dimensional (2D) MXenes have recently been shown to be promising for applications in anticancer photothermal therapy (PTT), owing to their outstanding photothermal performance. However, as with the other inorganic 2D nanomaterials, the MXene-based nanoplatforms lack the appropriate biocompatibility and stability in physiological conditions, targeting capability, and controlled release of drug, for cancer therapy. Fabricating a smart MXene-based nanoplatform for the treatment of cancer therefore remains a challenge. In this work, composite hydrogels based on cellulose and Ti3C2 MXene, were synthesized for the first time. We have shown that the cellulose/MXene composite hydrogels possess rapid response near-infrared-stimulated characteristics, which present as a continuous dynamic process in water. As a result, when loaded with the anticancer drug doxorubicin hydrochloride (DOX), the cellulose/MXene hydrogels are capable of significantly accelerating the DOX release. This behavior is attributed to the expansion of the pores within the three-dimensional cellulose-based networks, triggered by illumination with an 808 nm light. Capitalizing on their excellent photothermal performance and controlled, sustained release of DOX, the cellulose/MXene hydrogels are utilized as a multifunctional nanoplatform for tumor treatment by intratumoral injection. The results showed that the combination of PTT and prolonged adjuvant chemotherapy delivered using this nanoplatform was highly efficient for instant tumor destruction and for suppressing tumor relapse, demonstrating the potential of the nanoplatform for application in cancer therapy. Our work not only opens the door for the fabrication of smart MXene-based nanocomposites, along with their promising application against cancer, but also paves the way for the development of other inorganic 2D composites for applications in biomedicine.

Transparent, Adhesive, and Conductive Hydrogel for Soft Bioelectronics Based on Light-Transmitting Polydopamine-Doped Polypyrrole Nanofibrils

Abstract: Conductive hydrogels are promising materials for soft electronic devices. To satisfy the diverse requirement of bioelectronic devices, especially those for human–machine interfaces, hydrogels are required to be transparent, conductive, highly stretchable, and skin-adhesive. However, fabrication of a conductive-polymer-incorporated hydrogel with high performance is a challenge because of the hydrophobic nature of conductive polymers making processing difficult. Here, we report a transparent, conductive, stretchable, and self-adhesive hydrogel by in situ formation of polydopamine (PDA)-doped polypyrrole (PPy) nanofibrils in the polymer network. The in situ formed nanofibrils with good hydrophilicity were well-integrated with the hydrophilic polymer phase and interwoven into a nanomesh, which created a complete conductive path and allowed visible light to pass through for transparency. Catechol groups from the PDA–PPy nanofibrils imparted the hydrogel with self-adhesiveness. Reinforcement by the nanofibrils ...

On-Demand Dissolvable Self-Healing Hydrogel Based on Carboxymethyl Chitosan and Cellulose Nanocrystal for Deep Partial Thickness Burn Wound Healing.

Abstract: Deep partial thickness burn wounds present big challenges due to the long healing time, large size and irregular shape, pain and reinjury at wound dressing changes, as well as scarring. The clinically effective therapy to alleviate pain at wound dressing changes, and the scar left on the skin after the healing of wound is still unavailable. To combat this, we develop a nanocomposite self-healing hydrogel that can be injected into irregular and deep burn wound beds and subsequently rapidly self-heal to reform into an integrated piece of hydrogel that thoroughly fills the wound area and protects the wound site from external environment, finally being painlessly removed by on-demand dissolving using amino acid solution at wound dressing changes, which accelerates deep partial thickness burn wound healing and prevents scarring. The hydrogel is made out of naturally occurring polymers, namely, water-soluble carboxymethyl chitosan (CMC) and rigid rod-like dialdehyde-modified cellulose nanocrystal (DACNC). They are cross-linked by dynamic Schiff-base linkages between amines from CMC and aldehydes from DACNC. The large aspect ratio and specific surface area of DACNC raise massive active junctions within the hydrogel, which can be readily broken and reformed, allowing hydrogel to rapidly self-heal. Moreover, DACNC serves as nanoreinforcing fillers to improve the hydrogel strength, which also restricts the "soft" CMC chains' motion when soaked in aqueous system, endowing high fluid uptake capacity (350%) to hydrogel while maintaining integrity. Cytotoxicity assay and three-dimensional cell culture demonstrate excellent biocompatibility of the hydrogel and capacity as extracellular matrix to support cell growth. This work opens a novel pathway to fabricate on-demand dissolvable self-healing hydrogels to speed deep partial thickness burn wound healing and eliminate pain at wound dressing changes and prevent scar formation.

Cellulose-based hydrogel materials: chemistry, properties and their prospective applications

Abstract: Hydrogels based on cellulose comprising many organic biopolymers including cellulose, chitin, and chitosan are the hydrophilic material, which can absorb and retain a huge proportion of water in the interstitial sites of their structures These polymers feature many amazing properties such as responsiveness to pH, time, temperature, chemical species and biological conditions besides a very high-water absorption capacity Biopolymer hydrogels can be manipulated and crafted for numerous applications leading to a tremendous boom in research during recent times in scientific communities With the growing environmental concerns and an emergent demand, researchers throughout the globe are concentrating particularly on naturally derived hydrogels due to their biocompatibility, biodegradability and abundance Cellulose-based hydrogels are considered as useful biocompatible materials to be used in medical devices to treat, augment or replace any tissue, organ, or help function of the body These hydrogels also hold a great promise for applications in agricultural activity, as smart materials and some other useful industrial purposes This review offers an overview of the recent and contemporary research regarding physiochemical properties of cellulose-based hydrogels along with their applications in multidisciplinary areas including biomedical fields such as drug delivery, tissue engineering and wound healing, healthcare and hygienic products as well as in agriculture, textiles and industrial applications as smart materials

Highly Elastic and Ultratough Hybrid Ionic-Covalent Hydrogels with Tunable Structures and Mechanics.

Abstract: Hybrid ionically-covalently crosslinked double-network (DN) hydrogels are attracting increasing attention on account of their self-recovery ability and fatigue resistance, but their relative low mechanical strength and tedious performance adjustment severely limit their applications. Herein, a new strategy to concurrently fabricate hybrid ionic-covalent DN hydrogels and modulate their structures and mechanics is reported, in which an in situ formed chitosan ionic network is incorporated by post-crosslinking the chitosan-based composite hydrogel using multivalent anions solutions. The obtained hybrid DN hydrogels exhibit predominant mechanical properties including superior elastic modulus, high tensile strength, and ultrahigh fracture energy because of the more efficient energy dissipation of rigid short-chain chitosan network. Notably, the swollen hydrogels still remain mechanically strong and tough even after immersion in water for 24 h. More significantly, simply changing the post-crosslinking time can vary the compactness and rigidity of the chitosan network in situ, achieving flexible and efficient modulation of the structures and mechanics of the hybrid DN hydrogels. This study opens up a new horizon in the preparation and regulation of DN hydrogels for promising applications in tissue scaffolds, actuators, and wearable devices.