Crosslinker Concentration Research Articles

The Effect of Carbodiimide Crosslinkers on Gelatin Hydrogel as a Potential Biomaterial for Gingival Tissue Regeneration

Connective tissue grafts for gingival recession treatment present significant challenges as they require an additional surgical site, leading to increased morbidity, extended operative times, and a more painful postoperative recovery for patients. Gelatin contains the arginine–glycine–aspartic acid (RGD) sequence, which supports cell adhesion and interactions. The development of gelatin hydrogels holds significant promise due to their biocompatibility, ease of customization, and structural resemblance to the extracellular matrix, making them a potential candidate for gingival regeneration. This study aimed to assess the physical and biological properties of crosslinked gelatin hydrogels using EDC/NHS with two crosslinker concentrations (GelCL12 and GelCL24) and compare these to non-crosslinked gelatin. Both groups underwent morphological, rheological, and chemical analysis. Biological assessments were conducted to evaluate human gingival fibroblast (HGF) proliferation, migration, and COL1 expression in response to the scaffolds. The crosslinked gelatin group exhibited greater interconnectivity and better physical characteristics without displaying cytotoxic effects on the cells. FTIR analysis revealed no significant chemical differences between the groups. Notably, the GelCL12 group significantly enhanced HGF migration and upregulated COL1 expression. Overall, GelCL12 met the required physical characteristics and biocompatibility, making it a promising scaffold for future gingival tissue regeneration applications.

The e-Flower: A hydrogel-actuated 3D MEA for brain spheroid electrophysiology.

Traditional microelectrode arrays (MEAs) are limited to measuring electrophysiological activity in two dimensions, failing to capture the complexity of three-dimensional (3D) tissues such as neural organoids and spheroids. Here, we introduce a flower-shaped MEA (e-Flower) that can envelop submillimeter brain spheroids following actuation by the sole addition of the cell culture medium. Inspired by soft microgrippers, its actuation mechanism leverages the swelling properties of a polyacrylic acid hydrogel grafted to a polyimide substrate hosting the electrical interconnects. Compatible with standard electrophysiology recording systems, the e-Flower does not require additional equipment or solvents and is ready to use with preformed 3D tissues. We designed an e-Flower achieving a curvature as low as 300 micrometers within minutes, a value tunable by the choice of reswelling media and hydrogel cross-linker concentration. Furthermore, we demonstrate the ability of the e-Flower to detect spontaneous neural activity across the spheroid surface, demonstrating its potential for comprehensive neural signal recording.

Cross-Linker Architectures Impact Viscoelasticity in Dynamic Covalent Hydrogels.

Dynamic covalent cross-linked (DCC) hydrogels represent a significant advance in biomaterials for regenerative medicine and mechanobiology, offering viscoelasticity, and self-healing properties that more closely mimic in vivo tissue mechanics than traditional, predominantly elastic, covalent hydrogels. However, the effects of varying cross-linker architecture on DCC hydrogel viscoelasticity have not been thoroughly investigated. This study introduces hydrazone-based alginate hydrogels to explore how cross-linker architectures impact stiffness and viscoelasticity. In hydrogels with side-chain cross-linker (SCX), higher cross-linker concentrations enhance stiffness and decelerate stress relaxation, while an off-stoichiometric hydrazine-to-aldehyde ratio reduces stiffness and shortens relaxation time. In hydrogels with telechelic cross-linking, maximal stiffness and relaxation time occurs at intermediate cross-linker mixing ratio for both linear cross-linker (LX) and star cross-linker (SX), with higher cross-linker valency further enhancing these properties. Further, the ranges of stiffness and viscoelasticity accessible with the different cross-linker architectures are found to be distinct, with SCX hydrogels leading to slower stress relaxation relative to the other architectures, and SX hydrogels providing increased stiffness and slower stress relaxation versus LX hydrogels. This research underscores the pivotal role of cross-linker architecture in defining hydrogel stiffness and viscoelasticity, providing insights for designing DCC hydrogels with tailored mechanical properties for specific biomedical applications.

Formulation-Property Effects in Novel Injectable and Resilient Natural Polymer-Based Hydrogels for Soft Tissue Regeneration

The development of injectable hydrogels for soft tissue regeneration has gained significant attention due to their minimally invasive application and ability to conform precisely to the shape of irregular tissue cavities. This study presents a novel injectable porous scaffold based on natural polymers that undergoes in situ crosslinking, forming a highly resilient hydrogel with tailorable mechanical and physical properties to meet the specific demands of soft tissue repair. By adjusting the formulation, we achieved a range of stiffness values that closely mimic the mechanical characteristics of native tissues while maintaining very high resilience (>90%). The effects of gelatin, alginate, and crosslinker concentrations, as well as porosity, on the hydrogel’s properties were elucidated. The main results indicated a compression modulus range of 2.7–89 kPa, which fits all soft tissues, and gelation times ranging from 5 to 30 s, which enable the scaffold to be successfully used in various operations. An increase in gelatin and crosslinker concentrations results in a higher modulus and lower gelation time, i.e., a stiffer hydrogel that is created in a shorter time. In vitro cell viability tests on human fibroblasts were performed and indicated high biocompatibility. Our findings demonstrate that these injectable hydrogel scaffolds offer a promising solution for enhancing soft tissue repair and regeneration, providing a customizable and resilient framework that is expected to support tissue integration and healing with minimal surgical intervention.

Judd-Ofelt analysis and temperature sensing properties of polyethylmethacrylate (PEMA) networks doped with CdNb2O6: Er3+/Yb3+ phosphors

Research on the sensitivity of temperature measurements and optical thermometry involving rare earth ions has been an area of interest in the field of photonics and materials science. Introducing polymer networks as a new host material has an important role due to their properties including a versatile and stable environment for rare earth ions and rapid response in temperature detection. In this work, linear and crosslinked polyethylmethacrylate (PEMA) networks doped with Er3+/Yb3+ (1.5 mol % Er3+, 2 mol% Yb3+) synthesized by free-radical crosslinking polymerization with 0.1 EMA (weight %) at 60 °C were used to investigate direct and indirect optical bandgap energies and Urbach energy from UV–Visible spectra. The Judd-Ofelt (JO) approach was employed to analyze parameters Ωt (t = 2,4,6), spontaneous transition probabilities (Α), branching ratios (β) and radiative lifetimes (τ) as a function of linear and crosslinked PEMA doped nano-crystalline CdNb2O6: Er3+/Yb3+. The stimulated emission cross-sections of the transitions 2H11/2⟶4I15/2, 2S3/2⟶4I15/2 and 2F9/2⟶4I15/2 of Er3+/Yb3+ were calculated by two different methods; Fuchtbauer-Ladenburg formula and modified theory, respectively. The gain bandwidth cross-section product for the 2H11/2⟶4I15/2 was found to be 162.06. 10−28cm3, 260.94. 10−28cm3 and 461.20. 10−28cm3 of Er3+/Yb3+ embedded in linear, low and high crosslinked PEMA samples, respectively. JO parameters and stimulated emission cross-sections increased; therefore, radiative lifetimes decreased by increasing crosslinking content. In addition, the temperature dependence of upconversion (UC) luminescence was monitored under 975 nm excitation. The fluorescence intensity ratio (FIR) method examined the temperature sensing under two thermally coupled levels at 525 and 548 nm. The maximum sensitivities obtained from the FIR technique within the 300–650 K temperature range shifted to lower temperatures with increasing crosslinker content. Hence, linear and crosslinked polymer hosts doped rare-earth ions can be candidates for remote temperature sensors across various fields.

Curcumin-loaded lignin nanoparticles: Exploring sonication effects on drug loading and particle properties for future biomedical use

The present study investigates the effects of sonication and cross-linker (oxalic acid) concentration on drug loading and the properties of curcumin-loaded lignin nanoparticles. Selected samples were further assessed for their toxicity and antioxidant potential using the eukaryotic model organism Saccharomyces cerevisiae. Transmission electron microscopy analyses revealed the formation of spherical nanoparticles with diameters in the range of 39–49 nm. Differential scanning calorimetry experiments confirmed the encapsulation of curcumin. Factorial experimental design analyses indicated that sonication time, wave amplitude, cross-linker concentration, and their interactions significantly influenced both ζ-potential – from (−37.0 ± 1.7) mV to (−48.4 ± 0.6) mV – and curcumin loading – from (3.70 ± 0.32) % to (7.10 ± 0.57) %. These parameters are critical for biomedical applications as they relate to the clearance of nanoparticles from the human bloodstream and drug dosage optimization. Although sonication has been previously reported for the preparation of lignin nanoparticles, this study represents the first documented instance of manipulating drug loading by controlled sonication parameters. While none of the investigated factors significantly affected the mean particle diameter, observations from TEM micrographs suggest that cross-linker concentration and wave amplitude notably influence nanoparticle morphology. Moreover, the curcumin-loaded nanoparticles exhibited non-toxicity toward Saccharomyces cerevisiae and demonstrated the ability to enhance yeast cell tolerance to H2O2-induced oxidative stress, underscoring their antioxidant potential. Therefore, this research significantly contributes to the scientific understanding of how the control of sonication parameters and cross-linkers can modulate the properties of curcumin-loaded lignin nanoparticles for future biomedical applications.

Effect of particle stiffness on microgel self-assembly and suspension phase behavior over a broad temperature range

We synthesized thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) colloidal microgel particles of different stiffnesses by controlling the concentration of a polar crosslinker in a precipitation polymerization synthesis method. When suspended in an aqueous medium, the particles collapsed by expelling water as the temperature was raised toward the volume phase transition temperature (VPTT) of ≈ 34 °C. We noted that the sizes of the stiffer particles, synthesized with higher crosslinker concentration, collapsed less abruptly. Using Fourier transform infrared spectroscopy, we observed enhanced particle dehydration with increasing temperature and decreasing particle stiffness. Oscillatory rheology experiments on dense aqueous PNIPAM suspensions, prepared at a fixed particle effective volume fraction ϕeff = 1.5 at 25°C, revealed that suspensions constituted by the stiffest particles are the most elastic over a broad temperature range. Above the VPTT, suspensions of particles of intermediate stiffnesses exhibited two-step yielding, a typical signature of fragile gel formation. Zeta potential measurements showed that PNIPAM particles of lower stiffnesses are rendered electrostatically unstable in aqueous suspension. Combining cryogenic scanning electron microscopy and rheology, we noted a glass–glass transition when the temperature of a dense suspension of stiff PNIPAM particles was raised across the VPTT. In contrast, suspensions of particles of the lowest stiffnesses showed a gel-viscoelastic liquid–gel transition during an identical temperature ramp experiment. Our study reveals that temperature-induced phase transformations in dense PNIPAM suspensions depend sensitively on the stiffness of the constituent particles and can be explained by considering amphiphilicity-driven morphological changes in the suspension microstructures.

Influence of copper ion cross-linked CMC-PVA film on cell viability and cell proliferation study

In this study, films composed of carboxymethyl cellulose and polyvinyl alcohol were fabricated using the solution casting method. Citric acid (4 %) was employed as a cross-linking agent, while glycerol (3 %) as a plasticizer. Cupric chloride (CuCl2·2H2O) was used for cross-linking at concentrations 0.5 %, 1 %, and 3 % over different times. The cross-linking with copper ions led to a noticeable reduction in elasticity, with the breaking strain ranging from 17.9 %–52.9 %. The ion hydration phenomenon increased the contact angle and swelling ratio. Fourier-transform infrared (FTIR) spectroscopy confirmed esterification reactions and copper ion cross-linking with sodium carboxymethyl cellulose (Na-CMC). The films showed antibacterial activity against Staphylococcus aureus and Escherichia coli. The ion-released mechanism followed was the non-Fickian super case-II type. The concentration and duration of cross-linking significantly influenced cell viability and proliferation. FE-SEM analysis revealed that effective concentrations of CuCl2.2H2O were 0.5 % and 1 %, and cross-linking times were 5–15 min, facilitating cell attachment and proliferation. Films are non-adhesive with water vapor permeation 800–900 g/m2/day. These results indicate the potential use of the films in treating second-degree burn wounds with low to medium exudate levels. This study provides valuable insights into the development of copper-infused materials for advanced wound healing applications.

Biodegradable taro stem cellulose aerogel: A simple approach for adsorbing microplastics and dyestuffs contaminants

Water pollution and agricultural waste are pressing global issues. Herein, a biomass aerogel derived from waste taro stem microcrystalline cellulose (TS-MCC) was fabricated, in which, the effects of cellulose amount, cross-linker content, pre-freezing protocols on the aerogel’s property were studied. The optimized TS-MCC2.0 aerogel exhibited a hierarchical porous structure with good mechanical property (65.04 kPa) and adsorption capacities, with the qm towards microplastics (Polystyrene, PS) and dye (Congo red, CR) being 418.6 mg/g and 951.51 mg/g at 298 K, respectively. Meanwhile, it exhibited good applicability under different pH (3–11) and ionic strength environments, as well as the retained notably simultaneous adsorption ability even under mixed contaminant systems. The mathematical models suggested that the adsorption of PS and CR both fitted pseudo-second-order kinetics, and the adsorption isotherms could be described by the Langmuir and Freundlich models, respectively. Hydrogen bonding, electrostatic attraction, and π–π interactions were inferred as the main adsorption mechanisms towards PS and CR according to Fourier transform infrared spectrometer and X-ray photoelectron spectroscopy analysis. Moreover, the adsorption efficiencies were 92.37 % for PS and 88.34 % for CR after 5 reuse cycles. Therefore, this study provides a green aerogel sorbent for adsorbing microplastics and dyes contaminants.

Hydrogel System with Independent Tailoring of Mechanics, CT, and US Contrasts for Affordable Medical Phantoms.

Medical phantoms mimic aspects of procedures like computed tomography (CT), ultrasound (US) imaging, and surgical practices. However, the materials for current commercial phantoms are expensive and the fabrication with these is complex and lacks versatility. Therefore, existing material solutions are not suitable for creating patient-specific phantoms. We present a novel and cost-effective material system (utilizing ubiquitous sodium alginate hydrogel and coconut fat) with independently and accurately tailorable CT, US, and mechanical properties. By varying the concentration of alginate, cross-linker, and coconut fat, the radiological parameters and the elastic modulus were adjusted independently in a wide range. The independence was demonstrated by creating phantoms with features hidden in US, while visible in CT imaging and vice versa. This system is particularly beneficial in resource-scarce areas since the materials are cheap (<$ 1 USD/kg) and easy to obtain, offering realistic and versatile phantoms to practice surgeries and ultimately enhance patient care.

Self-Polymerized Tough and High-Entanglement Zwitterionic Functional Hydrogels.

Zwitterionic hydrogels exhibit great potential in biomedical applications due to their antifouling properties and biocompatibility. However, the single-network structure of pure zwitterionic hydrogels leads to a low toughness and strength, limiting their application in biomedical fields. In this work, a high entanglement sulfobetaine methacrylate-dopamine hydrogel (SBMA-DA-PE) with low cross-linker content and high monomer concentration is prepared by using a dopamine oxidative radical polymerization method. Compared to a regular zwitterionic hydrogel, the SBMA-DA-PE hydrogel exhibits a 5-fold increase in tensile fracture stress and a 10-fold increase in compressive fracture stress. The SBMA-DA-PE hydrogel possesses excellent mechanical properties (the maximum compressive stress ≥4.85MPa, the maximum compressive strain ≥90%). Besides, the non-covalent interactions between catechol or ortho-quinones within the SBMA-DA-PE hydrogel, combined with strong intermolecular electrostatic interactions, endow the SBMA-DA-PE hydrogel with great self-healing capabilities and fatigue resistance. The SBMA-DA-PE hydrogel demonstrates low swellability and possesses good antifouling properties. Furthermore, the good printability and conductivity of the tough SBMA-DA-PE hydrogel endows it with new possibilities for developing biological 3D scaffolds and electronic devices. Overall, this work provides new insights into the preparation of zwitterionic hydrogels with high mechanical strength and multi-functionality for biomedical applications.

Antimicrobial properties and biocompatibility of semi-synthetic carbohydrate-based ionic hydrogels.

Hydrogels have gained significant interest in the last decades, especially in the medical sector, due to their versatile properties. While hydrogels from naturally occurring polysaccharides (e.g. cellulose) are well-known, those produced from polymerizable carbohydrate-based monomers remain underexplored. However, these semi-synthetic hydrogels offer the great advantage of having adjustable properties for customization depending on their application. The objective of this study was to characterize semi-synthetic carbohydrate-based ionic hydrogels produced from GVIM-I (glucosyl vinyl imidazolium iodide). The antimicrobial activity was evaluated using the disk diffusion method, which demonstrated that all samples exhibit inhibitory effects on the growth of Candida auris. In vitro biocompatibility was determined by cell viability studies with L929 mouse fibroblasts, and a correlation was observed between eluate concentration and cell viability. In particular, the type of initiator system employed for polymerization was found to affect cell viability. The direct contact assessments showed that specific pre-treatments of the hydrogels resulted in higher cell viability than non-treated hydrogels. The results also revealed the impact of crosslinker concentration and type and identified poly(ethylene glycol)diacrylate (PEGDA) 575 as a promising crosslinker for future medical applications. LC-MS analysis of the wash medium identified unreacted GVIM-I as the leached material, which is presumed to be the cause of the observed cytotoxicity. Overall, the study provides valuable insights into the characteristics of GVIM-I based hydrogels and sheds light on the factors that influence their cytotoxicity and potential for medical application.

The Carrying Behavior of Water-Based Fracturing Fluid in Shale Reservoir Fractures and Molecular Dynamics of Sand-Carrying Mechanism

Water-based fracturing fluid has recently garnered increasing attention as an alternative oilfield working fluid for propagating reservoir fractures and transporting sand. However, the low temperature resistance and stability of water-based fracturing fluid is a significant limitation, restricting the fracture propagation and gravel transport. To effectively ameliorate the temperature resistance and sand-carrying capacity, a modified cross-linker with properties adaptable to varying reservoir conditions and functional groups was synthesized and chemically characterized. Meanwhile, a multifunctional collaborative progressive evaluation device was developed to investigate the rheology and sand-carrying capacity of fracturing fluid. Utilizing molecular dynamics simulations, the thickening mechanism of the modified cross-linker and the sand-carrying mechanism of the fracturing fluid were elucidated. Results indicate that the designed cross-linker provided a high viscosity stability of 130 mPa·s and an excellent sand-carrying capacity of 15 cm2 at 0.3 wt% cross-linker content. Additionally, increasing reservoir pressure exhibited enhanced thickening and sand-carrying capacities. However, a significant inverse relationship was observed between reservoir temperature and sand-carrying capacity, attributed to changes in the drag coefficient and thickener adsorption. These results verified the effectiveness of the cross-linker in enhancing fluid viscosity and sand-carrying capacity as a modified cross-linker for water-based fracturing fluid.

Design, synthesis, and characterization of novel copolymer gel particles for water-plugging applications

Abstract Multi-stage plugging represents a promising strategy for enhancing production and injection rates in medium-and low-permeability oilfields. Despite its potential, the efficacy of current plugging agents, particularly hydrophobically bonded water-soluble polyacrylamide-based gel microspheres, is hindered by notable drawbacks such as low stability and inadequate compressive strength. Therefore, a comprehensive understanding of water plugging mechanisms coupled with the optimization of gel microsphere properties is essential for advancing the development of gel-based plugging agents with superior characteristics or intelligent regulatory capabilities. The P(AA-AM-[PrSO3]Vim) ionic liquid copolymerized gel particles were designed and synthesized by using microfluidic technique and titration gel method with AM, acrylic acid (AA), 1-vinylimidazole (Vim) and 1,3-propylsulfonyl lactone (PrSO3) as the raw materials. The morphology and structure of the copolymer gel particles were characterized, and the effects of [PrSO3]Vim and cross-linker content on the water-absorbing properties and strength of the gel particles were investigated. When the amount of [PrSO3]Vim was 12%, the concentration of crosslinker was 1.5%, and the temperature was 40°C, the water absorption capacity reached the maximum value of 163 g·g−1. The strength of the P(AA–AM–[PrSO3]Vim) spherical gel particles was maximized at a [PrSO3]Vim content of 4%. Furthermore, the chemical and physical roles of the P(AA–AM–[PrSO3]Vim) spherical gel particles were studied in a typical water-plugging environment. This study provides experimental data and a theoretical basis for the application of functional spherical gel-plugging particles in current oilfield environments.

Enhanced stability and catalytic performance of immobilized phospholipase D on chitosan-encapsulated magnetic nanoparticles using oxidized dextran and glutaraldehyde as cross-linkers

Phospholipase D (PLD) is essential for the bioconversion of phosphatidylcholine (PC) to phosphatidylserine (PS), a process valuable in functional food and medicine. This study explores the stability and catalytic properties of PLD immobilized on chitosan-encapsulated magnetic nanoparticles (CMNPs), utilizing oxidized dextran (DX) and glutaraldehyde (Glu) as cross-linkers. The cross-linker concentration and immobilization time were optimized to assess their effects on PLD catalytic performance. PLD immobilized on CMNPs with DX (DX-CMNPs-PLD) exhibited optimal activity at pH 8.0 and 30 °C, retaining over 40 % activity after 14 cycles, while Glu-cross-linked PLD (Glu-CMNPs-PLD) retained approximately 65 %. DX-CMNPs-PLD demonstrated superior pH, temperature, and operational stability compared to free PLD. Additionally, the immobilized PLD was characterized using transmission electron microscopy, X-ray diffraction, and Fourier-transform infrared spectroscopy. Kinetics parameters (Vmax and Km) of the immobilized PLD were also studied with free PLD serving as a control. Conformational analyses indicated a significant change in PLD's secondary structure, particularly in β-sheet content, which likely contributed to the enhanced stability and activity. These findings suggest a promising approach for PLD immobilization on CMNPs, with notable implications for biotechnological applications.

Design of improved acellular fish skin as a promising scaffold for tissue regeneration applications

Decellularized marine tissues have been regarded as a desirable biomaterial because of their biological risk reduction, less religious constraints, and resemblance to mammalian tissues. The properties of these matrices can be improved by adding cross-linkers. In this study, after decellularization of the of Tilapia and Grass carp fish skin, a comparative study was conducted between them. Due to the higher abundance of collagen and glycosaminoglycans (GAGs) in Tilapia skin, it was selected for further study. In the next step, the cross-linking process was performed with three concentrations of 1-Ethyl-3-(3-dimethylaminopropyl) carbodiimide/ N-Hydroxysuccinimide (EDC/NHS) and tannic acid cross-linkers. The MTT results showed that the cross-linked samples with low concentrations of EDC/NHS had higher biocompatibility compared to the cross-linked sample with high concentration of EDC/NHS, as well as all samples cross-linked with tannic acid. Mechanical and physical studies conducted on the skin of Tilapia fish showed that the 15 mM/7.5 mM concentration of EDC/NHS increased the mechanical and temperature strength and decreased the degradability and it did not influence cell attachment.In general, it was shown that different fish skins differ in terms of collagen and GAGs, and the optimal concentration of EDC cross-linker improves the mechanical and physical properties of the matrix derived from fish skin.

Effects of crosslinker concentration on curing process and performances of needled fiber preform reinforced phenolic aerogel composite using process simulation and comprehensive experiments

A kind of needled quartz/carbon fiber preform reinforced phenolic aerogel composite (NQCF/PR) was fabricated through impregnating needled fiber preform with phenolic resin precursor solution, followed by sol–gel polymerization and solvent drying. The needled fiber preform serves as lightweight quasi-three-dimensional reinforcement, while phenolic aerogel matrix provides high porosity and low thermal conductivity. During fabrication of aerogel composite part using vacuum-assisted resin infusion process, distribution of crosslinker hexamethylenetetramine (HMTA) in precursor solution can be problematic, as precipitated crosslinker particles may be filtered by fibrous preform. In this study, the impact of HMTA filtration induced heterogeneous structure on subsequent curing process was investigated using process simulation. Temperature effects of sol–gel polymerization and solvent evaporation were considered through establishment of corresponding kinetic models. Impacts of heterogenous structure on distribution of temperature, resin curing degree and solvent conversion degree in large hemispherical aerogel composite structure were investigated. This leads to variations in gel network and pore structure of aerogel, thereby affecting final material performance. Based on experimental results, as HMTA concentration increases, compressive performance of NQCF/PR obviously increases. Among these, NQCF/PR with 4.7 wt% HMTA provides a balance of lightweight nature (0.25 g/cm3), excellent thermal insulation property (0.052 W·m−1·K−1) and compressive performance (strength of 0.35 MPa).

The effect of dynamic cross-links and mesogenic groups on the swelling and collapse of polymer gels

The polymer gels containing dynamic cross-links and mesogenic groups are among the key candidates for the development of soft actuators and detectors, displays, sensors and other programmable and self-healing materials. In this article, firstly, the collapse of polymer networks with irreversible cross-links in the presence of a dynamic cross-linker is investigated by means of Flory-type theory. It is shown that, at not a very poor solvent quality (near the theta-conditions), the swelling ratio for a gel containing irreversible and dynamic cross-links is less than for a gel with irreversible cross-links only, whereas at poor or good solvent qualities sizes of these gels are close to each other. The number of dynamic cross-links monotonically increases with worsening the solvent quality. The gel contraction can be also achieved by increasing the dynamic cross-linker concentration, which allows one to change the transition point in a wide range of solvent conditions. Secondly, polymer networks containing irreversible and dynamic cross-links and incorporating mesogenic side groups is studied using the Maier–Saupe theory. With decreasing in the temperature, the continuous transition from a swollen to collapsed state occurs. With further increase in the temperature, the swelling ratio discontinuously decreases and the nematic order parameter sharply increases from zero to a value ​​close to one. By increasing the dynamic cross-linker concentration, the swelling-to-collapse transition and, then, the isotropic-nematic transition are observed. A phase diagram of the gel is constructed and, depending on the dynamic cross-linker concentration and temperature, the swollen gel with the zero nematic order parameter, the collapsed gel with the zero nematic order parameter, and the collapsed gel with the nematic ordering can be formed. A growth of the length of the mesogenic side group leads to an increase in the area of ​​existence of the collapsed gel with the nematic ordering in the phase diagram. The obtained theoretical results are in agreement with corresponding experimental data from the literature.

Synthesis and Assessment of Acacia Gum‐Based Hydrogel as a Promising Novel Biopolymeric Matrix for Delivery of Ciprofloxacin

AbstractIn this current study, hydrogels based on acacia gum (AG), polyacrylamide (PAM), and carboxymethyl tamarind kernel gum (CMTKG) were successfully developed and ciprofloxacin (drug) incorporated into it. To optimize the hydrogel, the concentrations of crosslinker and initiator were varied, and their effects on the swelling were examined. The hydrogel was subjected to characterization techniques such as Powder X‐ray Diffraction (PXRD), Scanning Electron Microscopy (SEM), Attenuated Total Reflection‐Fourier Transform Infrared spectroscopy (ATR‐FTIR), and Thermogravimetric analysis (TGA). The hydrogel swelling and in vitro drug release were assessed in pH 1.2 and 7.4 buffer solutions. The findings revealed that an alkaline pH yielded superior results for the swelling and in vitro drug release experiments compared to an acidic pH. The drug release kinetic of the ciprofloxacin‐loaded AG/PAM/CMTKG hydrogel followed the Korsmeyer–Peppas model, demonstrating non‐fickian diffusion at pH 7.4 and fickian mechanism at pH 1.2. The pH‐dependent behavior of ciprofloxacin‐loaded AG/PAM/CMTKG hydrogel displayed its potential implications for site‐specific ciprofloxacin release.

Evaluation of phenolic compounds as cross-linkers to improve the qualities of halal gelatin from milkfish scales (Chanos chanos)

Gelatin is a versatile substance extensively used in medical and pharmaceutical industries for many applications, including capsule shells, X-ray film, infusion for plasma substitute, and the fabricating of artificial tissue. Fish scale gelatin is a profitable alternative source as a halal material despite its inferior quality. An addition of phenolic cross-linker may enhance the qualities of fish scale gelatin. The aim of this study was to determine the ability of phenolics to act as cross-linkers for fish scale gelatin and to identify the factors affecting this process. Gelatin production from fish scales (Chanos chanos) was carried out through basic pre-extraction and acidic pre-extraction. Thereafter, the gelatin was reacted with 10 different phenolics (phenol, pyrocatechol, resorcinol, α-naphthol, vanillin, L-tyrosine, curcumin, gallic acid, quercetin, and tannic acid). The resultant gelatins were characterized by infrared spectrum, X-ray diffraction pattern, swelling index, degree of cross-linking, viscosity, gel strength, mechanical profile, thermal profile, and water vapor permeability. Gelatin with the most favorable characteristics was further investigated for the effects of acidity (pH 4, 7, and 10) and cross-linker concentrations (2.5–10%). The findings revealed the formation of cross-linkage through shifted vibrational peaks of amide A, amide B, and amide II in the infrared spectrum. Shifted X-ray diffraction peaks in the gelatin with phenol addition also indicated the formation of cross-linkage. Significant improvement in the gelatin characteristics, such as swelling index, degree of cross-linking, viscosity, gel strength, mechanical profile, thermal profile, and water vapor permeability, could be attributed to the addition of phenolics cross-linkers. The highest improvement was observed in gelatin added with basic tannic acid 10%. Gelatin cross-linked with basic tannic acid 10% had a moisture content of 9.24±0.14%, swelling index of 323±17%, degree of cross-linking of 69.99±0.84%, viscosity of 8.48±0.23 cP, gel strength of 151.5±6.9 Bloom, melting temperature of 213.5°C, tensile strength of 7.00±0.54 N.cm-2, elongation at the break of 114.08±14.63%, elastic modulus of 58.45±8.20 N.cm-2 and water vapor permeability of 0.57±0.07 g.mm.m-2.h-1. kPa-1. The qualities of tannic acid-cross-linked gelatin films and film-forming gel increased when manufactured under basic conditions in comparison to acidic or neutral conditions. Furthermore, increasing the quantity of tannic acid to 10% improved the overall characteristics as compared to non-cross-linked gelatin. In conclusion, tannic acid has the ability to cross-link the fish gelatin, thereby enhancing its qualities.