Hydrogel Matrix Research Articles

Co-axial hydrogel spinning for facile biofabrication of prostate cancer-like 3D models

Glandular cancers are amongst the most prevalent types of cancer, which can develop in many different organs, presenting challenges in their detection as well as high treatment variability and failure rates. For that purpose, anticancer drugs are commonly tested in cancer cell lines grown in 2D tissue culture on plastic dishes in vitro, or in animal models in vivo. However, 2D culture models diverge significantly from the 3D characteristics of living tissues and animal models require extensive animal use and time. Glandular cancers, such as prostate cancer—the second leading cause of male cancer death—typically exist in co-centrical architectures where a cell layer surrounds an acellular lumen. Herein, this spatial cellular position and 3D architecture, containing dual compartments with different hydrogel materials, is engineered using a simple co-axial nozzle setup, in a single step utilizing prostate as a model of glandular cancer. The resulting hydrogel soft structures support viable prostate cancer cells of different cell lines and enable over-time maturation into cancer-mimicking aggregates surrounding the acellular core. The biofabricated cancer mimicking structures are then used as a model to predict the inhibitory efficacy of the poly ADP ribose polymerase inhibitor, Talazoparib, and the antiandrogen drug, Enzalutamide, in the growth of the cancer cell layer. Our results show that the obtained hydrogel constructs can be adapted to quickly obtain 3D cancer models which combine 3D physiological architectures with high-throughput screening to detect and optimize anti-cancer drugs in prostate and potentially other glandular cancer types.

A high-current hydrogel generator with engineered mechanoionic asymmetry.

Mechanoelectrical energy conversion is a potential solution for the power supply of miniaturized wearable and implantable systems; yet it remains challenging due to limited current output when exploiting low-frequency motions with soft devices. We report a design of a hydrogel generator with mechanoionic current generation amplified by orders of magnitudes with engineered structural and chemical asymmetry. Under compressive loading, relief structures in the hydrogel intensify net ion fluxes induced by deformation gradient, which synergize with asymmetric ion adsorption characteristics of the electrodes and distinct diffusivity of cations and anions in the hydrogel matrix. This engineered mechanoionic process can yield 4 mA (5.5 A m-2) of peak current under cyclic compression of 80 kPa applied at 0.1 Hz, with the transferred charge reaching up to 916 mC m-2 per cycle. The high current output of this miniaturized hydrogel generator is beneficial for the powering of wearable devices, as exemplified by a controlled drug-releasing system for wound healing. The demonstrated mechanisms for amplifying mechanoionic effect will enable further designs for a variety of self-powered biomedical systems.

A Review of Polymer-Based Environment-Induced Nanogenerators: Power Generation Performance and Polymer Material Manipulations.

Natural environment hosts a considerable amount of accessible energy, comprising mechanical, thermal, and chemical potentials. Environment-induced nanogenerators are nanomaterial-based electronic chips that capture environmental energy and convert it into electricity in an environmentally friendly way. Polymers, characterized by their superior flexibility, lightweight, and ease of processing, are considered viable materials. In this paper, a thorough review and comparison of various polymer-based nanogenerators were provided, focusing on their power generation principles, key materials, power density and stability, and performance modulation methods. The latest developed nanogenerators mainly include triboelectric nanogenerators (TriboENG), piezoelectric nanogenerators (PENG), thermoelectric nanogenerators (ThermoENG), osmotic power nanogenerator (OPNG), and moist-electric generators (MENG). Potential practical applications of polymer-based nanogenerator were also summarized. The review found that polymer nanogenerators can harness a variety of energy sources, with the basic power generation mechanism centered on displacement/conduction currents induced by dipole/ion polarization, due to the non-uniform distribution of physical fields within the polymers. The performance enhancement should mainly start from strengthening the ion mobility and positive/negative ion separation in polymer materials. The development of ionic hydrogel and hydrogel matrix composites is promising for future nanogenerators and can also enable multi-energy collaborative power generation. In addition, enhancing the uneven distribution of temperature, concentration, and pressure induced by surrounding environment within polymer materials can also effectively improve output performance. Finally, the challenges faced by polymer-based nanogenerators and directions for future development were prospected.

Synchronous semi-solid extrusion and photopolymerization of antimicrobial dressing hydrogel for wound healing

Bacterial infections at wound sites require more time for a fast and efficient wound-healing process. Antibacterial methyl cellulose-based hydrogel wound dressing can be an excellent option because it can show antibacterial action, absorb wound exudates, and have a cooling and soothing effect on the wound bed. The ultraviolet (UV) ray-assisted semi-solid extrusion 3D printing technique was used to prepare 3D printed construct into a high surface area mesh-like structure utilizing UV radiation for photocrosslinking of hydrogel matrix in the presence of Poly (ethylene glycol) Diacrylate. The prepared hydrogel was characterized for contact angle, and rheological analysis before semi-solid extrusion-based 3D printing. After optimization of printing parameters, the 3D printed mesh was subjected to physicochemical characterizations like dimensional analysis, swelling study, drug content, in vitro drug release, and in vitro antimicrobial activity study. A rheological analysis confirmed the viscosity, thixotropy, and viscoelastic nature of prepared hydrogel. Drug release study showed approximately 50 % release in 4 h, and >80 % drug release in 24 h. After optimization of one batch, hydrogel polymerization was done by functional group analysis followed by validation of thread thickness by electron microscopy images and mechanical property assessment. The 3D-printed mesh was further evaluated for its in-vitro antibacterial performance against Escherichia coli and Staphylococcus aureus. The area of inhibition was one-fold more in Staphylococcus aureus and two-fold in E. coli, ensuring diffusion of the drug from 3D printed mesh and killing of bacteria. The work reported herein represents a universal platform to generate multifunctional and customized hydrogels with various functional substances for wound dressing applications.

In situ sono-rheometric assessment of procaine-loaded calcium pectinate hydrogel for enhanced drug releasing under ultrasound stimulation

Ultrasound (US) triggered alterations in the viscoelastic behavior of the procaine-loaded ionically gelatinized pectin hydrogel matrix, and drug release was observed using a sono-device rheometer. The gel softened immediately upon activation of the ultrasound operated at 43 kHz and remained in a softened state throughout the irradiation. Upon cessation of ultrasound, the gel promptly reverted to its original hardness. This cycle of softening was consistently observed in ionically crosslinked pectin hydrogels, resulting in the promotion of procaine release, particularly with higher US power and lower calcium concentration. As the amount of loaded procaine increased, the gel weakened due to ion exchange with the calcium crosslinker and procaine. The most substantial release efficiency, reaching 82 % with a concentration of 32 μg/ml, was achieved when the hydrogels contained 0.03 % procaine within the gelatinized hydrogel medicine at a calcium concentration of 0.9 M, representing a six-fold increase compared to that without US. Notably, US exposure affected the 3D porous structure and degradation rate, leading to hydrogel collapse and facilitating medicine release. Additionally, the procaine-loaded pectin hydrogels with 0.9 M calcium exhibited improved fibroblast cell viability, indicating non-toxicity compared to those hydrogels prepared at a higher Ca2+ concentration of 2.4 M.

Preparation of environmentally friendly, high strength, adhesion and stability hydrogel based on lignocellulose framework

Hydrogels are extensively utilized in the fields of electronic skin, environmental monitoring, biological dressings due to their excellent flexibility and conductivity. However, traditional hydrogel materials possess drawbacks such as environmental toxicity, low strength, poor stability, and water loss deactivation, which limited its frequent applications. Here, a flexible conductive hydrogel called wood-based DES hydrogel (WDH) with high strength, high adhesion, high stability, and high sensitivity was successfully synthesized by using environmentally friendly lignocellulose as skeleton and deep eutectic solvent as matrix. The strength of WDH prepared from lignocellulose framework is approximately 50 times higher than poly deep eutectic solvent hydrogel, and about 4.5 times higher than that prepared from cellulose skeleton. The WDH exhibits stable adhesion to most common materials and demonstrates exceptional dimensional stability. Its conductivity remains unaffected by water, even after prolonged exposure to air, maintaining a value of 0.0245 S/m. The anisotropy inherent in the system results in three distinct linear sensing intervals for WDH, exhibiting a maximum sensitivity of 5.45. This paper verified the advantages of lignocellulose framework in improving the strength and stability of hydrogels, which provided a new strategy for the development of sensor materials.

Transition from active motion to anomalous diffusion for Bacillus subtilis confined in hydrogel matrices

We investigate the motility of B. subtilis under different degrees of confinement induced by transparent porous hydrogels. The dynamical behavior of the bacteria at short times is linked to characteristic parameters describing the hydrogel porosity. Mean squared displacements (MSDs) reveal that the run-and-tumble dynamics of unconfined B. subtilis progressively turns into sub-diffusive motion with increasing confinement. Correspondingly, the median instantaneous velocity of bacteria decreases and becomes more narrowly distributed, while the reorientation rate increases and reaches a plateau value. Analyzing single-trajectories, we show that the average dynamical behavior is the result of complex displacements, in which active, diffusive and sub-diffusive segments coexist. For small and moderate confinements, the number of active segments reduces, while the diffusive and sub-diffusive segments increase. The alternation of sub-diffusion, diffusion and active motion along the same trajectory can be described as a hopping ad trapping motion, in which hopping events correspond to displacements with an instantaneous velocity exceeding the corresponding mean value along a trajectory. Different from previous observations, escape from local trapping occurs for B. subtilis through active runs but also diffusion. Interestingly, the contribution of diffusion is maximum at intermediate confinements. At sufficiently long times transport coefficients estimated from the experimental MSDs under different degrees of confinement can be reproduced using a recently proposed hopping and trapping model. Finally, we propose a quantitative relationship linking the median velocity of confined and unconfined bacteria through the characteristic confinement length of the hydrogel matrix. Our work provides new insights for the bacterial motility in complex media that mimic natural environments and are relevant to important problems like sterilization, water purification, biofilm formation, membrane permeation and bacteria separation.

Cannabidiol-loaded microparticles embedded in a porous hydrogel matrix for biomedical applications

In this study, poly (lactic-co-glycolic acid) (PLGA) microparticles loaded with cannabidiol (CBD) were synthesized (PLGA@CBD microparticles) and embedded up to 10 wt% in a chondroitin sulfate/polyvinyl alcohol hydrogel matrix. In vitro chemical, physical, and biological assays were carried out to validate the potential use of the modified hydrogels as biomaterials. The microparticles had spherical morphology and a narrow range of size distribution. CBD encapsulation efficiency was around 52%, loading was approximately 50%. Microparticle addition to the hydrogels caused minor changes in their morphology, FTIR and thermal analyses confirmed these changes. Swelling degree and total porosity were reduced in the presence of microparticles, but similar hydrophilic and degradation in phosphate buffer solution behaviors were observed by all hydrogels. Rupture force and maximum strain at rupture were higher in the modified hydrogels, whereas modulus of elasticity was similar across all materials. Viability of primary human dental pulp cells up to 21 days was generally not influenced by the addition of PLGA@CBD microparticles. The control hydrogel showed no antimicrobial activity against Staphylococcus aureus, whereas hydrogels with 5% and 10% PLGA@CBD microparticles showed inhibition zones. In conclusion, the PLGA@CBD microparticles were fabricated and successfully embedded in a hydrogel matrix. Despite the hydrophobic nature of CBD, the physicochemical and morphological properties were generally similar for the hydrogels with and without the CBD-loaded microparticles. The data reported in this study suggested that this original biomaterial loaded with CBD oil has characteristics that could enable it to be used as a scaffold for tissue/cellular regeneration.Graphical

Modulating the release of bioactive molecules of human mesenchymal stromal cell secretome: Heparinization of hyaluronic acid-based hydrogels

An amine derivative of hyaluronic acid (HA) was crosslinked to obtain a 3D dried sponge. The sponge was subsequently rehydrated using secretome from human mesenchymal stromal cells (MSCs), resulting in the formation of a hydrogel. The release kinetics analysis demonstrated that the hydrogel effectively sustained secretome release, with 70% of the initially loaded wound-healing-associated cytokines being released over a 12-day period. Tuning the hydrogel properties through heparin crosslinking resulted in a biomaterial with a distinct mechanism of action. Specifically, the presence of heparin enhanced water uptake capacity of the hydrogel and increased its sensitivity to enzymatic degradation. Notably, the heparin crosslinking also led to a significant retention of cytokines within the hydrogel matrix. Overall, the secretome-rehydrated HA hydrogel holds promise as a versatile device for regenerative medicine applications: the non-heparinized hydrogel may function as a biomaterial with low reabsorption rates, sustaining the release of bioactive molecules contained in MSC secretome. In contrast, the heparinized hydrogel may serve as a depot of bioactive molecules with faster reabsorption rates. Given its patch-like characteristic, the HA-based hydrogel appears suitable as topical treatment for external organs, such as the skin.

Self-Healing Hydrogel Bioelectronics.

Hydrogels have emerged as powerful building blocks to develop various soft bioelectronics because of their tissue-like mechanical properties, superior bio-compatibility, the ability to conduct both electrons and ions, and multiple stimuli-responsiveness. However, hydrogels are vulnerable to mechanical damage, which limits their usage in developing durable hydrogel-based bioelectronics. Self-healing hydrogels aim to endow bioelectronics with the property of repairing specific functions after mechanical failure, thus improving their durability, reliability, and longevity. This review discusses recent advances in self-healing hydrogels, from the self-healing mechanisms, material chemistry, and strategies for multiple properties improvement of hydrogel materials, to the design, fabrication, and applications of various hydrogel-based bioelectronics, including wearable physical and biochemical sensors, supercapacitors, flexible display devices, triboelectric nanogenerators (TENGs), implantable bioelectronics, etc. Furthermore, the persisting challenges hampering the development of self-healing hydrogel bioelectronics and their prospects are proposed. This review is expected to expedite the research and applications of self-healing hydrogels for various self-healing bioelectronics.

A stimuli-responsive hydrogel for reversible information storage, encryption and decryption

Smart hydrogel materials, known for their sensitivity to external stimuli, exhibit a reversible dynamic response and find applications in diverse fields, particularly in information storage. Despite significant efforts in this domain, developing a hydrogel with high-resolution, repeatable recording, and robust information encryption/decryption capabilities still remains a challenge. In this study, we synthesized a polymer hydrogel, namely polyvinyl alcohol-n-isopropylacrylamide-octadecyl polyoxyethylene ether acrylate hydrogel (PPNS), which features multiple hydrogen bonds through copolymerization, by using N-isopropylacrylamide, polyvinyl alcohol, and octadecyl polyoxyethylene ether acrylate (SGA15) as raw materials. The PPNS hydrogel demonstrated outstanding high-resolution, repeatable recording capabilities, enabling reversible recording, encryption, and decryption of information using anhydrous ethanol as the inducer. Varying the SGA15 monomer concentration revealed that the PPNS-2% hydrogel, prepared with 2% SGA15, outperformed the other hydrogels in terms of information recording and encryption/decryption when immersed in anhydrous ethanol and deionized water. Furthermore, the PPNS-2% hydrogel exhibited the ability to undergo multiple information cycles while maintaining excellent mechanical properties even after 25 cycles. Notably, ethanol served as a specialized ink for inscribing different patterns on the hydrogel surface for information recording. The recorded information could be erased through water wiping or ethanol volatilization, enabling reversible information recording, encryption, and decryption. Due to their responsive and dynamic nature of PPNS hydrogels are positions them as promising candidates for use as innovative information storage platforms.

Reconfigurable Growth of Engineered Living Materials.

The growth of multicellular organisms is a process akin to additive manufacturing where cellular proliferation and mechanical boundary conditions, among other factors, drive morphogenesis. Engineers have limited ability to engineer morphogenesis to manufacture goods or to reconfigure materials comprised of biomass. Herein, a method that uses biological processes to grow and regrow magnetic engineered living materials (mELMs) into desired geometries is reported. These composites contain Saccharomyces cerevisiae and magnetic particles within a hydrogel matrix. The reconfigurable manufacturing process relies on the growth of living cells, magnetic forces, and elastic recovery of the hydrogel. The mELM then adopts a form in an external magnetic field. Yeast within the material proliferates, resulting in 259 ± 14% volume expansion. Yeast proliferation fixes the magnetic deformation, even when the magnetic field is removed. The shape fixity can be up to 99.3 ± 0.3%. The grown mELM can recover up to 73.9 ± 1.9% of the original form by removing yeast cell walls. The directed growth and recovery process can be repeated at least five times. This work enables ELMs to be processed and reprocessed into user-defined geometries without external material deposition.

A Flexible and Free‐Standing Photonic Crystal‐Hydrogel Film for Enhanced Fluorescence from Nitrogen Doped Carbon Dots

AbstractEnhancement of fluorescence emission in a flexible and free‐standing fluorescing film is a key requirement for sensing platforms with augmented sensitivity. In this context, a study on the enhanced fluorescence emission from nitrogen‐doped carbon dots (NCDs) embedded on a flexible free‐standing photonic crystal hydrogel film prepared via photopolymerization, is presented. The composite structure utilizes the photonic crystal enhanced fluorescence (PCEF) technique and incorporates a self‐assembled 3D photonic crystal (3D PC) onto a photopolymerizable hydrogel matrix containing the NCDs. The 3D PC template is prepared through vertical deposition self‐assembly using monodisperse polystyrene (PS) spheres. By leveraging the enhanced excitation and extraction effect in a PC‐fluorophore composite, the authors’ structure exhibits a fourfold enhancement in fluorescence emission compared to the control sample. The relative positioning of the photonic stopband with the excitation and emission spectra of the fluorophore (NCDs) is thoroughly studied by selecting four different 3D PCs with varied lattice parameters. In addition, the hydrogel matrix offers improved photostability and enhanced lifetime for the NCDs. This structure can be further modified into an efficient sensor through appropriate functionalization.

Accelerating the remodeling of collagen in cutaneous full-thickness wound using FIR soldering technology with bio-targeting nanocomposites hydrogel.

A novel composite wound dressing hydrogel by incorporating single-walled carbon nanotubes and indocyanine green into a dual-crosslinked hydrogel through Schiff base reaction was developed. The objective was to prevent wound infection and enhance the thermal effect induced by laser energy. The hydrogel matrix was constructed using oxidized gelatin, pre-crosslinked with calcium ions, along with carboxymethyl chitosan, crosslinked via Schiff base reaction. Optimization of the blank hydrogel's gelation time, swelling index, degradation rate, and mechanical properties was achieved by adding 0.1% SWCNT and 0.1% ICG. Among them, the SWCNT-loaded hydrogel BCG-SWCNT exhibited superior performance overall: a gelation time of 102 s; a swelling index above 30 after equilibrium swelling; a degradation rate of 100.5% on the seventh day; and a compressive modulus of 8.8 KPa. It displayed significant inhibition against methicillin-resistant Staphylococcus aureus infection in wounds. When combined with laser energy usage, the composite hydrogel demonstrated excellent pro-healing activity in rats.

Piezoelectric Hydrogels: Hybrid Material Design, Properties, and Biomedical Applications.

Hydrogels show great potential in biomedical applications due to their inherent biocompatibility, high water content, and resemblance to the extracellular matrix. However, they lack self-powering capabilities and often necessitate external stimulation to initiate cell regenerative processes. In contrast, piezoelectric materials offer self-powering potential but tend to compromise flexibility. To address this, creating a novel hybrid biomaterial of piezoelectric hydrogels (PHs), which combines the advantageous properties of both materials, offers a systematic solution to the challenges faced by these materials when employed separately. Such innovative material system is expected to broaden the horizons of biomedical applications, such as piezocatalytic medicinal and health monitoring applications, showcasing its adaptability by endowing hydrogels with piezoelectric properties. Unique functionalities, like enabling self-powered capabilities and inducing electrical stimulation that mimics endogenous bioelectricity, can be achieved while retaining hydrogel matrix advantages. Given the limited reported literature on PHs, here recent strategies concerning material design and fabrication, essential properties, and distinctive applications are systematically discussed. The review is concluded by providing perspectives on the remaining challenges and the future outlook for PHs in the biomedical field. As PHs emerge as a rising star, a comprehensive exploration of their potential offers insights into the new hybrid biomaterials.

Photo-Controlled Reversible Uptake and Release of a Modified Sulfamethoxazole Antibiotic Drug from a Pillar[5]arene Cross-Linked Gelatin Hydrogel.

Pillararene cross-linked gelatin hydrogels were designed and synthesized to control the uptake and release of antibiotics using light. A suite of characterization techniques ranging from spectroscopy (FT-IR, 1H and 13C NMR, and MAS NMR), X-ray crystallographic analysis, scanning electron microscopy (SEM), and thermogravimetric analysis (TGA) was employed to investigate the physicochemical properties of hydrogels. The azobenzene-modified sulfamethoxazole (Azo-SMX) antibiotic was noncovalently incorporated into the hydrogel via supramolecular host-guest interactions to afford the A-hydrogel. While in its ground state, the Azo-SMX guest has a trans configuration structure and forms a thermodynamically stable inclusion complex with the pillar[5]arene motif in the hydrogel matrix. When the A-hydrogel was exposed to 365 nm UV light, Azo-SMX underwent a photoisomerization reaction. This changed the structure of Azo-SMX from trans to cis, and the material was released into the environment. The Azo-SMX released from the hydrogel was effective against both Gram-positive and Gram-negative bacteria. Importantly, the A-hydrogel exhibited a striking difference in antibacterial activity when applied to bacterial colonies in the presence and absence of UV light, highlighting the switchable antibacterial activity of A-hydrogel aided by light. In addition, all hydrogels containing pillar[5]arenes have demonstrated biocompatibility and effectiveness as scaffolds for biological and medical purposes.

Hydrogel-Based Skin Regeneration.

The skin is subject to damage from the surrounding environment. The repair of skin wounds can be very challenging due to several factors such as severe injuries, concomitant infections, or comorbidities such as diabetes. Different drugs and wound dressings have been used to treat skin wounds. Tissue engineering, a novel therapeutic approach, revolutionized the treatment and regeneration of challenging tissue damage. This field includes the use of synthetic and natural biomaterials that support the growth of tissues or organs outside the body. Accordingly, the demand for polymer-based therapeutic strategies for skin tissue defects is significantly increasing. Among the various 3D scaffolds used in tissue engineering, hydrogel scaffolds have gained special significance due to their unique properties such as natural mimicry of the extracellular matrix (ECM), moisture retention, porosity, biocompatibility, biodegradability, and biocompatibility properties. First, this article delineates the process of wound healing and conventional methods of treating wounds. It then presents an examination of the structure and manufacturing methods of hydrogels, followed by an analysis of their crucial characteristics in healing skin wounds and the most recent advancements in using hydrogel dressings for this purpose. Finally, it discusses the potential future advancements in hydrogel materials within the realm of wound healing.

Thermally exfoliated graphene oxide doped microporous bio-nanocomposite hydrogel: A promising substrate for biomedical application

Hydrogels have demonstrated significant promise as flexible/wearable sensors for the diagnosis, monitoring, and delivery of personalized medicine for health issues and deficiencies. To this end, a novel approach was employed towards the development of a hybrid hydrogel nanocomposite-based biosensing substrate. The hierarchical hydrogel matrix derived by using polyaniline (PANI)/polyvinyl-alcohol (PVA) biopolymer-matrix, was reinforced with in-house synthesized thermally exfoliated graphene-oxide (TEGO). Fourier transform infrared spectroscopy (FT-IR) confirmed the interfacial-interactions between hydroxyl groups and functional groups of TEGO, a conducive property for immobilization and catalytic activities. X-ray photoelectron spectroscopy (XPS) investigation of the developed nanocomposite hydrogel demonstrated that the addition of nanofiller facilitated the ordered structure of nanocomposite hydrogel. Further, field emission scanning electron microscopy (FE-SEM) investigations revealed interconnected porous microstructure of the nanocomposites, assisted by nucleating effect of TEGO, a supporting micro-environment for the transportation of biomolecules. Impedance analysis and hall effect studies showed that the nanocomposite hydrogel substrate was highly conductive. In vitro cytocompatibility results demonstrated excellent biocompatibility of the bio-nanocomposite hydrogels. Cyclic-voltammetry analysis indicated a reduction in current on the surface due to long-range shattered conjugated network of TEGO and PANI in presence of functional groups. Overall, this study indicates that developed bio-nanocomposite hydrogel substrates are promising candidates for biomedical applications.

In Situ Polymerization of Hydrogel Electrolyte on Electrodes Enabling the Flexible All-Hydrogel Supercapacitors with Low-Temperature Adaptability.

All-hydrogel supercapacitors are emerging as promising power sources for next-generation wearable electronics due to their intrinsic mechanical flexibility, eco-friendliness, and enhanced safety. However, the insufficient interfacial adhesion between the electrode and electrolyte and the frozen hydrogel matrices at subzero temperatures largely limit the practical applications of all-hydrogel supercapacitors. Here, an all-hydrogel supercapacitor is reported with robust interfacial contact and anti-freezing property, fabricated by in situ polymerizing hydrogel electrolyte onto hydrogel electrodes. The robust interfacial adhesion is developed by the synergistic effect of a tough hydrogel matrix and topological entanglements. Meanwhile, the incorporation of zinc chloride (ZnCl2) in the hydrogel electrolyte prevents the freezing of water solvents and endows the all-hydrogel supercapacitor with mechanical flexibility and fatigue resistance across a wide temperature range of 20°C to -60°C. Such all-hydrogel supercapacitor demonstrates satisfactory low-temperature electrochemical performance, delivering a high energy density of 11mWhcm-2 and excellent cycling stability with a capacitance retention of 90% over 10000 cycles at -40°C. Notably, the fabricated all-hydrogel supercapacitor can endure dynamic deformations and operate well under 2000 tension cycles even at -40°C, without experiencing delamination and electrochemical failure. This work offers a promising strategy for flexible energy storage devices with low-temperature adaptability.

Investigation of nanocomposite PNIPAm‐g‐graphene with pre‐lower critical solution temperature rapid thermal response function for chip adaptive cooling: A molecular dynamics and computational fluid dynamics simulations

AbstractTemperature‐sensitive hydrogels have been widely used for rapid adaptive cooling in electronic device thermal management with promising applications. However, existing temperature‐sensitive hydrogels can only regulate the flow in the chip cooling system after the ambient temperature reaches their lower critical solution temperature (LCST). Before reaching LCST, effective rapid heat dissipation for electronic chips is not achievable. This study aims to develop a temperature‐sensitive hydrogel that can provide assisted adaptive cooling for electronic chips before reaching its LCST. This requires the hydrogel to have a thermal conductivity far surpassing existing hydrogel materials. Using the temperature‐sensitive hydrogel PNIPAm and graphene molecules as base materials, this research utilized molecular dynamics simulations to graft graphene molecules onto PNIPAm molecules in different ways, resulting in the temperature‐sensitive hydrogel material PNIPAm‐g‐graphene. Non‐equilibrium molecular dynamics (NEMD) was employed to calculate the thermal conductivity of this material under different temperature conditions. The results indicate that the thermal conductivity of PNIPAm‐g‐graphene can reach up to 1.95474 W/m K (graphene grafted at CH3 functional group, temperature at 280 K). Compared to the thermal conductivity of PNIPAm under the same conditions (0.45 W/m K), the increase in thermal conductivity is significant, demonstrating excellent thermal conductivity compared to PNIPAm. Subsequently, this study analyzed the underlying mechanisms of different thermal conductivities in materials obtained by grafting graphene molecules at different points using the method of overlap in Phonon Density of States Curves (PDOS) from the perspective of interfacial thermal conduction. Finally, through computational fluid dynamics (CFD) simulations, this study investigates the chip's adaptive cooling performance with PNIPAm‐g‐graphene material. The results show that, compared to traditional temperature‐sensitive hydrogels, PNIPAm‐g‐graphene can achieve efficient adaptive cooling of chip hotspots before the cooling fluid temperature reaches its LCST value. This finding is significant for the field of chip cooling. The study proposes a new method for rapid, adaptive cooling of chip hotspots and explores its feasibility from the perspectives of molecular dynamics and CFD simulation. It holds importance in the thermal management of electronic devices and the rapid adaptive cooling of electronic chips.