Cross-linked Gel Research Articles

In-Situ Cross-linked F- and P-Containing Solid Polymer Electrolyte for Long-Cycling and High-Safety Lithium Metal Batteries with Various Cathode Materials.

The practical application of lithium metal batteries (LMBs) has been hindered by limited cycle-life and safety concerns. To solve these problems, we develop a novel fluorinated phosphate cross-linker for gel polymer electrolyte in high-voltage LMBs, achieving superior electrochemical performance and high safety simultaneously. The fluorinated phosphate cross-linked gel polymer electrolyte (FP-GPE) by in-situ polymerization method not only demonstrates high oxidation stability but also exhibits excellent compatibility with lithium metal anode. LMBs utilizing FP-GPE realize stable cycling even at a high cut-off voltage of 4.6 V (vs Li/Li+) with various high-voltage cathode materials. The LiNi0.6Co0.2Mn0.2O2|FP-GPE|Li battery exhibits an ultralong cycle-life of 1200 cycles with an impressive capacity retention of 80.1 %. Furthermore, the FP-GPE-based batteries display excellent electrochemical performance even at practical conditions, such as high cathode mass loading (20.84 mg cm-2), ultrathin Li (20 μm), and a wide temperature range of -25 to 80 °C. Moreover, the first reported solid-state 18650 cylindrical LMBs have been successfully fabricated and demonstrate exceptional safety under mechanical abuse. Additionally, the industry-level 18650 cylindrical LiMn2O4|FP-GPE|Li4Ti5O12 cells demonstrate a remarkable cycle-life of 1400 cycles. Therefore, the impressive electrochemical performance and high safety in practical batteries demonstrate a substantial potential of well-designed FP-GPE for large-scale industrial applications.

Effect of Starch Types on the Textural and Rehydration Properties of Extruded Peanut Protein Pore Gel Particles.

In this study, the effect of different starches from corn, potato and pea containing varying amylose/amylopectin ratios on the textural and rehydration properties of extruded peanut protein gel particles were investigated. Results showed that textural and rehydration properties of peanut protein extruded with corn starch, potato starch and amylopectin are slightly inferior to those of peanut protein with pea starch extrudates. The addition of pea starch led to an increase in the pore structure of the peanut protein extrudates and improved their water absorption index, simultaneously reducing the hardness and density. Pea starch, as a natural water-absorbing expansion material, helped peanut protein to form cross-linked gel polymers that bind more water molecules, in addition to further polymerization with peanut protein, which made the protein secondary structure became disordered. These changes directly affected the textural properties of the extrudates. In addition, the blended system of starches and peanut protein tended to form more elastic solids, which affected the expansion of the extrudates. These findings indicate that starch can effectively improve the poor expansion of proteins, making it suitable for use in the production of plant protein-based foods.

Use of Limestone Sludge in the Preparation of ɩ-Carrageenan/Alginate-Based Films.

The use of processed limestone sludge as a crosslinking agent for films based on Na-alginate and ɩ-carrageenan/Na-alginate blends was studied. Sorbitol was tested as a plasticizer. The produced gel formulations included alginate/sorbitol and carrageenan/alginate/sorbitol mixtures, with tested sorbitol concentrations of 0.0, 0.5 and 1.0 wt%. The limestone sludge waste obtained from the processing of quarried limestone was converted into an aqueous solution of Ca2+ by dissolution with mineral acid. This solution was then diluted in water and used to induce gel crosslinking. The necessity of using sorbitol as a component of the crosslinking solution was also assessed. The resulting films were characterized regarding their dimensional stability, microstructure, chemical structure, mechanical performance and antifungal properties. Alginate/sorbitol films displayed poor dimensional stability and were deemed not viable. Carrageenan/alginate/sorbitol films exhibited higher dimensional stability and smooth and flat surfaces, especially in compositions with 0.5 wt% sorbitol. However, an increasing amount of plasticizer appears to result in severe surface cracking, the development of a segregation phenomenon affecting carrageenan and an overall decrease in films' mechanical resistance. Although further studies regarding film composition-including plasticizer fraction, film optimal thickness and film/mold material interaction-are mandatory, the attained results show the potential of the reported ɩ-carrageenan/alginate/sorbitol films to be used towards the development of viable films derived from algal polysaccharides.

Evaluating the Efficacy and Safety of Hemofence (Thorombin Cross-Linked Sodium Hyaluronate Gel Matrix) in Hemostasis for Intractable Exudative Bleeding in Spinal Surgery: A Multicenter, Randomized, Phase III Clinical Trial.

To demonstrate the noninferiority of the novel hemostatic agent, Hemofence (BMI Korea Co., Ltd., thrombin cross-linked sodium hyaluronate gel matrix) compared to the established agent, Floseal Hemostatic Matrix (Baxter, thrombin-gelatin matrix) in achieving hemostasis for spinal surgeries, with secondary objectives to assess additional efficacy and safety. This clinical trial was a multicenter, randomized, subject-blinded, active-controlled, parallel-group, phase 3 study. Investigational drugs were administered to the first and second bleeding sites of each participant (or only to the first site if a second site was absent), evaluating hemostasis success rate within 10 minutes and the time to achieve hemostasis. Subsequent visits were conducted for safety assessments. For noninferiority test, a 97.5% one-sided confidence interval (CI) was used; the test group was deemed noninferior if the lower limit exceeded -10%. This trial showed a 97.10% success rate in the test group and 96.05% in the control group for primary efficacy. The 95% CI (-4.90% to 7.44%) confirmed the test drug's noninferiority. Time to hemostasis showed no significant difference between groups. All adverse events, adverse drug reactions, and serious adverse events were statistically similar between groups (p=1.000, p=0.243, and p=0.966, respectively). A novel hemostatic agent, Hemofence, demonstrated an efficacy and safety profile comparable to that of Floseal.

Enhancing the Quality of Low-Salt Silver Carp (Hypophthalmichthys molitrix) Surimi Gel Using Psyllium Husk Powder: An Orthogonal Experimental Approach.

Low-salt surimi production is crucial as it addresses health concerns related to sodium intake while maintaining the quality and shelf-life of seafood products. This research focused on optimizing the gelation conditions for silver carp surimi with the addition of psyllium husk powder at low salt concentrations (0.5% and 1%, w/w) to investigate the effects of psyllium husk powder concentration, temperature, and time on gel strength and water-holding capacity. The quality was assessed in terms of gel strength and water-holding capacity. Following a single-factor exploration, a three-level orthogonal experiment was designed to evaluate the influence of these three variables using a combined scoring system. Results indicated that psyllium husk powder levels between 0.1% and 0.3% (w/w) enhanced gel strength and water-holding capacity. The optimal conditions were identified as follows: 1% (w/w) NaCl with 0.2% (w/w) psyllium husk powder for 2.5 h at 35 °C, and 0.5% (w/w) NaCl with 0.3% (w/w) psyllium husk powder for 3 h at 35 °C. Texture profile analysis revealed that psyllium husk powder increased the hardness of the surimi gel, promoting myosin cross-linking and denser gel structure. Compared to traditional surimi gel, which relies on ionic bonds, the optimized gel showed higher levels of disulfide cross-linking and enhanced hydrophobic interactions, resulting in a stronger gel structure. Sensory evaluation suggested that surimi gels with psyllium husk powder were perceived as better than those without psyllium husk powder. The study concludes that selecting the appropriate psyllium husk powder quantity and thermal processing conditions based on salt concentration can significantly improve the quality of low-salt surimi gels. Error analysis using one-way ANOVA was performed on all experimental data and (p < 0.05) indicated the significant difference.

Effect of glycosylation on soy protein isolate–sodium carboxymethyl cellulose conjugates heat-induced gels and their applications as carriers of riboflavin

The objective of this study was to improve the rheological properties and riboflavin delivery ability of soy protein isolate (SPI) gels by incorporating sodium carboxymethyl cellulose (CMC) through glycosylation. The investigation focused on the structural and gel properties of SPI–CMC conjugates at different Maillard reaction times (30, 60, 90, 120, and 150 min). The results showed that the degree of grafting initially increased and then decreased as the Maillard reaction times increased, reaching its peak at 90 min (25.52%). The changes in the structure and conformation of the SPI–CMC conjugates were verified by Fourier transform infrared spectroscopy and surface hydrophobicity. An appropriate Maillard reaction reduced the content of highly ordered α-helix and β-sheet while increasing the content of disordered random coil and β-turn. This secondary structural change led to protein unfolding, exposure of surface hydrophobic groups, and orderly aggregation, forming a dense cross-linked gel network. When the Maillard reaction times increased, especially for 90 min, the gel strength and water-holding capacity of the SPI–CMC conjugate gels were significantly increased, along with a denser microstructure. Compared with the SPI and SPI–CMC mixture, SPI–CMC conjugate gels with 60 and 90 min reaction times exhibited notably increased viscosity and storage modulus (G′), as well as better structural recovery characteristics. The above physicochemical property improvements markedly enhanced the riboflavin encapsulation efficiency and riboflavin delivery ability of SPI–CMC conjugate gels, improving the ability to protect riboflavin from photodegradation and slowly releasing riboflavin in the simulated intestinal environment. Hence, SPI–CMC conjugate gels have significant potential for the delivery of nutrients.

Engineering heterogeneous hierarchical hydrogels based on Artemisia sphaerocephala Krasch polysaccharide/whey protein isolate fibrils aqueous two-phase emulsion

Emulsion-templating techniques have been used to develop structurally anisotropic hydrogels. This paper proposes a method to couple biopolymer assembly behavior with a phase-separated aqueous two-phase system (ATPS) to construct a hierarchical structure on protein-polysaccharide hydrogels. Based on the phase separation of Artemisia sphaerocephala Krasch polysaccharide (ASKP) and whey protein isolate (WPI) fibrils, a bi-continuous hydrogel was fabricated through spontaneous iron-facilitated molecular chelation. The impact of WPI fibrils under ultrasonic treatment for varying durations on gel structurization and physicochemical properties was also exploited. Shorter length of WPI fibrils facilitated stepwise cross-linking gelation during the oxidation of ferrous ions to ferric ions. Specifically, ultrasonic treatment for 6 min and 8 min promoted the accumulation of shorter fibrils, resulting in the formation of a more intensive clockwise-oriented hierarchical network. Compared to the hydrogels with longer linear aggregates without the ultrasonic treatment, the incorporation of the shorter aggregates resulting from ultrasonic treatment for 6 min and 8 min significantly increased the gel's water holding capacity and mechanical properties. Additionally, the fibrils that underwent ultrasonic treatment for 6 min resulted in a more stable three-dimensional network with optimal elastic performance. This study presents a new water-in-water emulsion-templated strategy for structural regulation and stabilization of multiform hydrogel.

An in-situ cross-linked network PMMA-based gel polymer electrolyte with excellent lithium storage performance

Gel polymer electrolytes (GPEs) effectively combine the advantages of high ionic conductivity and reduce the risk of leakage associated with liquid. In this study, a chemically cross-linked gel polymer electrolyte was prepared by in-situ polymerization using polymethyl methacrylate (PMMA) as a matrix and neopentyl glycol diacrylate (NPGDA) as cross-linking agent. The cross-linked structure of the GPE was preliminarily investigated, as well as the influence of the degree of cross-linking on its physical properties. The GPE exhibited a superior conductivity of 1.391 mS cm−1 at 25 °C. Herein, the Li|GPE|LiNi0.8Co0.1Mn0.1O2 cell has an excellent capacity retention rate of 80.7% after 150 cycles at 0.5 C in addition to a high discharge specific capacity of 203 mAh g−1. The structure of the cathode material is shielded from the production of byproducts during the charging and discharging of lithium-ion batteries by the cross-linked PMMA GPE.

Multistep pH-peak-focusing liquid chromatography with a hydrophilic polymer gel column for separation of rare earth elements

Multistep pH-peak-focusing liquid chromatography with a column packed with a hydrophilic polymer gel (a cross-linked hydroxylated methacrylic polymer gel) was developed for separation of rare earth metal ions. Metal ions in a sample solution introduced to the column are chromatographically extracted into the stationary gel phase at the top of the column equilibrated with a basic solution used as the first mobile phase containing acetylacetone and 1,10-phenanthroline by synergistic extraction effect. After the sample solution is introduced, the mobile phases are delivered into the column by stepwise gradient elution in order of decreasing pH. Each metal ion is concentrated at a pH border formed between the zones of different pH in the column and moves toward the outlet of the column with the pH border. Mutual separation of La(III), Ce(III), Nd(III), Eu(III), Y(III), Tb(III), and Yb(III) was achieved by the present method for an 1-mL sample injection with the column of which the inner volume is 11.8 mL. The multistep pH-peak-focusing liquid chromatography with a hydrophilic polymer gel column developed in this study has great potential as a useful method for the separation of rare earth metal ions on a preparatory scale.

Modulation of sodium distribution and digestion properties in low salt myofibrillar protein gel incorporating γ-polyglutamic acid and transglutaminase: Conformation and microstructure

The weak gelling and poor digestion properties of myofibrillar protein (MP) under low-salt conditions constrain the development of functional sodium-reduced meat products. This study investigated how modification with γ-polyglutamic acid (γ-PGA) and transglutaminase (TG) cross-linking influences the conformation, gelation, and in vitro digestion of low-salt MPs pretreated with konjac glucomannan (KGM) and ultrasound. The results revealed that γ-PGA addition effectively facilitated the exposure of tryptophan and tyrosine residues in low salt MPs. The better dispersibility and slightly lower rheological properties of protein sols suggested the circumscribed effect of γ-PGA in augmenting protein gelation. TG crosslinking promoted moderate aggregation of MPs through different sites in myosin fragments, augmented the uniform distribution of sodium, and remarkably enhanced the gelling behavior of MPs. Importantly, the simultaneous incorporation of γ-PGA contributed to the refinement and uniformization of the TG cross-linked protein gel network, especially in the protein gel modified by pre-ultrasound treatment in combination with KGM. This result could also be corroborated by the augmented intermolecular interactions and enhanced digestibility observed in γ-PGA-modified TG crosslinked protein gel. Coupled with the identification of potentially bioactive peptides, it was confirmed that myosin light chain, actin, and myomesin account for the major contribution to the γ-PGA-induced changes in MP gels. Therefore, TG cross-linking combined with γ-PGA could be used to regulate the conformation and gelling properties of low-salt MPs, thus influencing the sodium distribution and digestion properties of low-salt meat products.

Fast-relaxing hydrogels with reversibly tunable mechanics for dynamic cancer cell culture

The mechanics of the tumor microenvironment (TME) significantly impact disease progression and the efficacy of anti-cancer therapeutics. While it is recognized that advanced in vitro cancer models will benefit cancer research, none of the current engineered extracellular matrices (ECM) adequately recapitulate the highly dynamic TME. Through integrating reversible boronate-ester bonding and dithiolane ring-opening polymerization, we fabricated synthetic polymer hydrogels with tumor-mimetic fast relaxation and reversibly tunable elastic moduli. Importantly, the crosslinking and dynamic stiffening of matrix mechanics were achieved in the absence of a photoinitiator, often the source of cytotoxicity. Central to this strategy was Poly(PEGA-co-LAA-co-AAPBA) (PELA), a highly defined polymer synthesized by reversible addition-fragmentation chain transfer (RAFT) polymerization. PELA contains dithiolane for initiator-free gel crosslinking, stiffening, and softening, as well as boronic acid for complexation with diol-containing polymers to give rise to tunable viscoelasticity. PELA hydrogels were highly cytocompatible for dynamic culture of patient-derived pancreatic cancer cells. It was found that the fast-relaxing matrix induced mesenchymal phenotype of cancer cells, and dynamic matrix stiffening restricted tumor spheroid growth. Moreover, this new dynamic viscoelastic hydrogel system permitted sequential stiffening and softening to mimic the physical changes of TME.

3D Cellulose‐Based Solar Evaporator with Tunable Porous Structures for High Steam Generation

AbstractSolar vapor evaporation have emerged as a promising green technology to harvest fresh water. Achieving high evaporation rates while employing accessible and renewable materials is key focus in this field. Here, a 3D cylindrical‐shaped solar evaporator composed of natural cellulose is fabricated through ice‐templating freezing combined with crosslinking gelation. It demonstrates an evaporation rate of 4.2 kg m−2 h−1 under 1 sun irradiation, and reaches an energy efficiency of 173%, surpassing most reported cellulose/wood‐based evaporators. This enhanced performance is facilitated by absorbing energy from surrounding, possessing connected pores, and reducing the evaporation enthalpy. Moreover, a systematic exploration of the correlation between pore size and evaporation performance reveals that the reduced pore size (several micrometers) does not necessarily result in a higher evaporation rate, despite improving the fluid transportation. The interaction between water and cellulose induces the formation of intermediate water and reduces the evaporation enthalpy by more than 35%. Thus, the final evaporation performance is determined by a synergistic effect involving water transport, hydrophilicity, and vaporization enthalpy. Giving the high evaporation rate achieved, this 3D cellulose‐based solar evaporator presents a promising candidate toward a high‐throughput, eco‐friendly solar steam generation devices, aligning well with the criteria of green and sustainable development.

Improved stability and mechanical properties of citrus pectin-zein emulsion gels by double crosslinking with calcium and transglutaminase

The low water solubility of zein severely limits its industrial application. In this study, the emulsifying performance and stability of zein were improved by electrostatically compounding different ratios of citrus pectin (CP) with zein to obtain zein-CP composite particles (ZCPs). When the mass ratio of CP to zein was 1: 2 (C1Z2), the composite particles showed the smallest particle size, and the C1Z2 stabilized Pickering emulsion (C1Z2-PE) exhibited excellent physical and environmental stability. The ZCPs stabilized emulsions were further cross-linked by transglutaminase (TGase) and Ca2+, resulting in the formation of emulsion gels with increased mechanical properties. Macroscopic and microscopic morphology analysis demonstrated the successful preparation of the emulsion gels. Through the rheological study and texture analysis, it was observed that the double cross-linked emulsion gels exhibited a remarkable improvement in apparent viscosity and gel hardness. This research offers a new strategy and technical reference for the development of new gel-based products.

Biomimetic hybrid porous microspheres with plant membrane-wall structure for evaluating multiscale mechanisms of ultrasound-assisted mass transfer

Determination of mass transfer during ultrasound-assisted extraction (UAE) has always been a challenge, not to mention the novel breakthrough of mechanisms for its positive effects. Herein, versatile porous microspheres (PM) with membrane-wall structure like plant tissues, which were made from sodium alginate/polyacrylamide dual crosslinking gels loaded with liposomes, were prepared to reveal the micro mass transfer effects during UAE. Results showed that prepared PM kept stable microstructure during extraction and ultrasound significantly accelerated the pore diffusion rather than surface diffusion. This effect resulted in higher UAE efficiency of PM with 60 % porosity than solid microspheres (143.72 to 155.47 mg/L), and the finding can be further explained as the accelerated internal diffusion (14.25 %) under ultrasound treatment. Moreover, multi-physics coupling simulations were performed to elucidate the enhanced pore flow and UAE efficiency. Acoustic streaming induced by cavitation effect increased the seepage velocity within the PM, and the pore structure would undergo compression and expansion deformation with alternated acoustic pressure due to its elastic characteristic. Both microscale effects improved the mass transfer and increase the UAE efficiency without structural damage from cavitation. This study fills the UAE mechanisms from micro view and provides a novel method for the study of vital micro processes.

Laboratory evaluation of high-temperature resistant lysine-based polymer Gel systems for leakage control

In-situ crosslinking gel known for its cost-effectiveness, has been employed for decades to plug high-permeability features in subsurface environments. However, some commonly used crosslinkers are being phased out due to the increasingly rigorous environmental regulations. As a newly discovered environmentally friendly crosslinker, lysine can crosslink the partially hydrolyzed polyacrylamide through transamidation reaction. The present work aimed to study the effect of polymer composition and concentration on the gelation behavior of lysine and high molecular weight acrylamide-based polymers. Several commercial high molecular weight polymers with different contents of 2-Acrylamido-2-methyl-1-propane sulfonic acid (AMPS) including AN-105/125, SAV-55/37/28, and SAV-10 were deployed in this work. High-temperature/pressure-resistant glass tubes were used to study the crosslinking behavior. The plugging efficiency test used a high permeability sandstone core (1600 mD). Besides, the effect of salinity and pH on the crosslinking behavior, gel strength, and long-term thermal stability was also studied. Results showed that increasing the AMPS content could prolong the gelation time, but the polymer and lysine mixture failed to form gels when the AMPS content was excessively high. Additionally, increasing the AMPS content negatively affects the gel strength but positively impacts long-term thermal stability. Polymer gel with a relatively high content of AMPS could be stable in 0.5 % CaCl2 solution at 130 °C for over 200 days. The polymer/lysine gel system can efficiently plug the high permeability matrix, and the plugging efficiency is higher than 99 %. The polymer/lysine gel system is a promising green leakage control system in treating the high conductivity features in geothermal and oil reservoirs.

Secondary Chemical Cross-Linking to Improve Mechanical Properties in a Multifaceted Biocompatible Strain Sensor.

A new conductive and transparent organohydrogel is developed with high stretchability, excellent mechanical, self-healing, antifreezing, and adhesive properties. A simple one-pot polymerization method is used to create polyacrylamide cross-linked through N,N'-methylenebis(acrylamide) (MBAA) and divinylbenzene (DVB). The dual chemical cross-linked gel network is complemented by several physical cross-links via hydrogen bonding and π-π interaction. Multiple chemical and physical cross-links are used to construct the gel network that allows toughness (171 kPa), low modulus (≈45 kPa), excellent stretchability (>1100%), and self-healing ability. The use of appropriate proportions of the water/glycerol binary solvent system ensures efficient environment tolerance (-20 to 40 °C). Phytic acid is used as a conductive filler that provides excellent conductivity and contributes to the physical cross-linking. Dopamine is incorporated in the gel matrix, which endows excellent adhesive property of the gel. The organohydrogel-based strain sensors are developed with state-independent properties, highly linear dependence, and excellent antifatigue performance (>100 cycles). Moreover, during the practical wearable sensing tests, human motions can be detected, including speaking, smiling, and joint movement. Additionally, the sensor is biocompatible, indicating the potential applications for the next generation of epidermal sensors.

Comparison of Structural, Water-Retaining and Sorption Properties of Acrylamide-Based Hydrogels Cross-Linked by Physical and Chemical Methods.

Two series of hydrogels based on acrylamide and its copolymers with acrylonitrile and acrylic acid were synthesized by two cross-linking methods - chemical (using N,N'-methylene bis-acrylamide) and physical (using montmorillonite (MMT)) ones. The structure of the gels was characterized by Fourier Transform Infrared spectroscopy (FTIR) and scanning electron microscopy (SEM). The swelling and sorption properties were analyzed as a function of both the monomer composition and the cross-linking method. The shift of the band corresponding to Si-O (995-1030 cm-1 ) confirmed the formation of intercalation structures for MMT-cross-linked gels. Moreover, physically cross-linked gels demonstrated a non-monotonic dependence of the swelling degree on the MMT concentration, and acrylamide-acrylic acid copolymer MMT-cross-linked gels showed pH sensitivity and the highest swelling degree of 150 g/g. The highest sorption capacity towards cadmium(II) ions was demonstrated by acrylamide-acrylic acid copolymer gels, both covalently cross-linked (30 mg/g) and MMT-cross-linked (8.9 mg/g).

Thermokinetic and Chemorheology of the Geopolymerization of an Alumina-Rich Alkaline-Activated Metakaolin in Isothermal and Dynamic Thermal Scans.

Alkaline sodium hydroxide/sodium silicate-activating high-purity metakaolin geopolymerization is described in terms of metakaolin deconstruction in tetrahedral hydrate silicate [O[Si(OH)3]]- and aluminate [Al(OH)4]- ionic precursors followed by their reassembling in linear and branched sialates monomers that randomly copolymerize into an irregular crosslinked aluminosilicate network. The novelty of the approach resides in the concurrent thermo-calorimetric (differential scanning calorimetry, DSC) and rheological (dynamic mechanical analysis, DMA) characterizations of the liquid slurry during the transformation into a gel and a structural glassy solid. Tests were run either in temperature scan (1 °C/min) or isothermal (20 °C, 30 °C, 40 °C) cure conditions. A Gaussian functions deconvolution method has been applied to the DSC multi-peak thermograms to separate the kinetic contributions of the oligomer's concurrent reactions. DSC thermograms of all tested materials are well-fitted by a combination of three overlapping Gaussian curves that are associated with the initial linear low-molecular-weight (Mw) oligomers (P1) formation, oligomers branching into alumina-rich and silica-rich gels (P2), and inter- and intra-molecular crosslinking (P3). The loss factor has been used to define viscoelastic behavioral zones for each DMA rheo-thermogram operated in the same DSC thermal conditions. Macromolecular evolution and viscoelastic properties have been obtained by pairing the deconvoluted DSC thermograms with the viscoelastic behavioral zones of the DMA rheo-thermograms. Two main chemorheological behaviors have been identified relative to pre- and post-gelation separation of the viscoelastic liquid from the viscoelastic solid. Each comprises three behavioral zones, accounting for the concurrently occurring linear and branching oligomerization, aluminate-rich and silica-rich gel nucleations, crosslinking, and vitrification. A "rubbery plateau" in the loss factor path, observed for all the testing conditions, identifies a large behavioral transition zone dividing the incipient gelling liquid slurry from the material hard setting and vitrification.

A strong nucleophilic fluorination agent to achieve highly stable in-situ 3D cross-linked gel polymer electrolyte for lithium-ion batteries

The Gel Polymer Electrolyte (GPE) is recognized as a promising alternative to conventional electrolytes, aiming to enhance the longevity and energy density of lithium-ion batteries (LIBs). However, several challenges persist, particularly concerning the conductivity and voltage window of GPE in battery systems. In this study, we introduce an in-situ 3D crosslinked GPE, using polymethyl methacrylate (PMMA) as the monomer and polyethylene glycol dimethacrylate (PEGDMA) as the crosslinking agent, to ensure structural stability and optimized ion conductivity. We also incorporate a potent nucleophilic fluorination agent, Tetrabutylammonium fluoride (TBAF), to augment the compatibility and oxidation resistance of the formulated FGPPE. The recurring (–CH2CH2O-) units of PEGDMA, coupled with in-situ lithium fluoride (LiF) and C-F groups introduced by TBAF, endow the FGPPE with a remarkable ionic conductivity of 7.8 mS cm−1 and a distinctly electrochemical stability of 4.65 V. Notably, the Li metal anode, featuring an F-rich solid-state interface (SEI), demonstrates uniform Li+ deposition, sustaining a cycling life of 1000 h and maintaining a commendable average coulomb efficiency of 98.5 % over 300 cycles. Additionally, the NCM811/SiC pouch cell integrated with FGPPE showcases superior cycling stability, retaining 99.4 % of its capacity after 600 cycles at an elevated voltage of 4.45 V. Such advancements in gel polymer electrolyte design can significantly expedite the commercial deployment of gel polymer Li-ion batteries.

Long-Term Follow-Up of the Behavior of Facial Volumizing Cross-Linked Hyaluronic Acid Gels

Introduction: We present the long-term follow-up photographic and MRI data on 4 patients 42-44 months after cross-linked Hyaluronic Acid (HA) gel injection into the temple region. All injected HA gels were produced using the registered and patented “Inter Penetration Network Like®” (IPN-Like® cross-linking technology) (LABORATOIRES VIVACY, France). The initial results following injection and up to 24 months were previously reported [1,2]. Material and methods: Our study population comprised 4 Caucasian patients who were enrolled into our two previous studies that compared Stylage XL versus Stylage XL-Lido (incorporating lidocaine added at manufacturing) [1] and Stylage XL versus Stylage XXL [2]. Patients, radiologists and the independent evaluators were blinded to the type of product used. The 4 patients were each injected in both temporal fossae using the 2 different HA gels being compared (one on either side). All patients had their follow-up at month 42 after injection (M42) with the exception of one patent who her MRI and photographs taken at the same setting on month 44 (M44). Photographic assessments were undertaken by the injector and 2 independent experts using Merz-Analogic Scale® (MAS®) and the Global Aesthetic Improvement Scale (GAIS). Results: Except for participant 2 (Stylage® XL vs. Stylage® XL-Lido) on the Stylage® XL-Lido side, all the other participants were considered to have a degree of persisting improvement compared to baseline, according to experts scoring of photographs on MAS and GAIS, However, there was a gradual deterioration in the level of improvement compared to the other assessment time-points. MRI: Although the bolus of injected gel was spherical at D0, we observed a change in the shape of the implant over time on MRI, where it changed from a round to a “teardrop” shape. Slow resorption occurred from 18 months onwards. At M42-44, the gel appearance on MRI remained similar to that previously reported at M18. The MRI residual volume calculation showed persistent increased volume compared to the volume initially injected. The product location appeared stable. There were no radiological or clinical signs of inflammatory reaction in tissues adjacent to the gel. Conclusion: At long-term follow-up 42-44 months after initial injection there was still an improvement in the aesthetic appearance of the temporal fossa and the MRI images show the continued presence of the gel. We also noticed that Stylage®XL (without lidocaine) seemed to absorb more water than its counterpart with lidocaine. Likewise, Stylage® XL seemed to absorb more water than Stylage® XXL.