Hydrophobic Association Research Articles

Hydrophobic Association Hydrogel Enabled by Multiple Noncovalent Interactions for Wearable Bioelectronics in Amphibious Environments

Hydrophobic Association Hydrogel Enabled by Multiple Noncovalent Interactions for Wearable Bioelectronics in Amphibious Environments

In-silico Design, ADMET Screening, Prime MM-GBSA Binding Free Energy Calculation and MD Simulation of Some Novel Phenothiazines as 5HT6R Antagonists Targeting Alzheimer's Disease.

Alzheimer's disease is a type of dementia that affects neuronal function, leading to a decline in cognitive functions. Serotonin-6 (5HT6) receptors are implicated in the etiology of neurological diseases. 5HT6 receptor antagonists act as anti-dementia agents. 7YS6 represents a membrane protein, and amplification and overexpression of this protein are associated with Alzheimer's disease. Coumarin-fused phenothiazines are significant anti-Alzheimer's agents due to their inhibitory activity on the Serotonin- 6 receptor. Numerous previously unreported Coumarin-substituted Phenothiazines [A2 to A50] were designed using in-silico methods to evaluate their 5HT6 receptor antagonistic activity. Molecular modeling techniques were employed to study the ligands [A2 to A50] in interaction with the Serotonin-6 receptor (PDB ID: 7YS6) using Schrödinger Suite 2019-4. Molecular modeling studies of the designed ligands [A2 to A50] were conducted using the Glide module. In-silico ADMET screening was performed using the QikProp module, and binding free energy calculations were carried out using the Prime MM-GBSA module within the Schrödinger Suite. The binding affinity of the designed ligands [A2 to A50] towards 5HT6 receptors was determined based on Glide scores. Subsequently, ligand A31 underwent a 100 ns molecular dynamics simulation using the Desmond module of Schrödinger Suite 2020-1, which is based in New York, NY. The majority of the designed ligands exhibited strong hydrogen bonding interactions and hydrophobic associations with the serotonin-6 receptor, which hinder its activity. These ligands achieved remarkable Glide scores within the range of -4.2859 to -7.7128, in comparison to reference standards such as Idalopirdine (-7.78149), Intepirdine (-5.20103), Latrepirdine (-5.54853), and the co-crystallized ligand (-7.02889). In-silico ADMET properties for these ligands fell within the recommended values for drug-likeness. It is worth noting that the MM-GBSA binding free energy of the most potent inhibitor was positive, indicating a strong binding interaction. Additionally, the dynamic behavior of the protein (7YS6)-ligand (A31) complex was studied by subjecting ligand A31 to a 100 ns molecular dynamics simulation. The results of this study reveal strong evidence supporting the potential of coumarin- substituted phenothiazine derivatives as effective Serotonin-6 receptor antagonists. Ligands [A2 to A50], which exhibited noteworthy Glide scores, hold promise for significant anti- Alzheimer activity. Further in-vitro and in-vivo investigations are warranted to explore and confirm their therapeutic potential.

PH-Induced Mechanical Transition in Polyion Complex Hydrogels: Shifting from Ionic Association to Hydrophobic Association

pH-Induced Mechanical Transition in Polyion Complex Hydrogels: Shifting from Ionic Association to Hydrophobic Association

The characteristics and flocculation performance of hydrophobic association poly‐(3‐methacryloylamido propyl trimethyl ammonium chloride)

AbstractThe cationic polymer plays a crucial role in the flocculation process for solid–liquid separation. A hydrophobic‐associated cationic polymer was prepared through micellar free‐radical polymerization of cationic monomer 3‐methyl acrylamide propyl trimethyl ammonium chloride (MAPTAC) and hydrophobic monomer Poly (ethylene glycol) Octadecyl methacrylate (OEMA). The Poly‐MAPTAC‐OEMA can form network structure through intermolecular hydrophobic association in aqueous solution, which leads to the solution viscosity increase and the salt thickening property. The critical associating concentrations (CACs) of Poly‐MAPTAC‐OEMA are 5818–6992 mg/L in aqueous solution. For the diatomite suspensions, at the dosage above about 5 mg/L, the Poly‐MAPTAC‐OEMA can show higher flocculation efficiency compared with Poly‐MAPTAC. Specifically, at the dosage of 8 mg/L, the enhancement rate of sedimentation rate can reach 7.27%–32.31%. Meanwhile, the hydrophobic association mainly enhances the bridging ability but has no significant effect on the improvement of the electric neutralization ability of Poly‐MAPTAC‐OEMA. The flocculation performance‐enhanced dosage of Poly‐MAPTAC‐OEMA is obviously lower than the CAC of Poly‐MAPTAC‐OEMA; this may be because during the flocculation process, the Poly‐MAPTAC‐OEMA first absorb and deeply concentrate on the particle surface, and then the hydrophobic association and bridging enhancement of Poly‐MAPTAC‐OEMA can occur more easily on the particle surface.

A stiff and tough triple-shape memory hydrogel triggered at body temperature by hydrophobic association and electrostatic interaction

While triple-shape memory hydrogels (TSMHs) are considered promising materials for intelligent medical devices, obtaining TSMHs triggered at the human body temperature with adequate mechanical performance remains challenging. Herein, a stiff and tough TSMH with a wide glass transition temperature (Tg) range at approximately 36 °C is constructed by copolymerizing hydrophobic 2-aminoethyl methacrylate isopropyl carbamate (IMA) with zwitterionic sulfobetaine methacrylate (SBMA). While the introduction of SBMA into the poly(2-aminoethyl methacrylate isopropyl carbamate) (PIMA) polymer chain weakens the ultra-strong hydrophobic association, it causes an electrostatic interaction, which increases the flexibility of the copolymer chains and the cross-linking density of the network. Based on these structural characteristics, the poly(2-aminoethyl methacrylate isopropyl carbamate-co- sulfobetaine methacrylate) [P(IMA-co-SBMA)] hydrogels show reasonable triple shape memory effect with wide Tg ranging from 22 °C to 46 °C, Young's modulus from 2.82 MPa to 22.15 MPa, and fracture strain from 43 % to 444 %. This study provides a novel strategy for balancing the mechanical properties and Tg of TSMHs as materials for intelligent medical devices.

Polyionic liquid ionogels formed via hydrophobic association for flexible strain sensors

A series of self-healing polyionic liquid ionogels based on hydrophobic association were designed and fabricated for application in strain sensors.

Network interactions simultaneously enhance stiffness and lubricity of triple-network hydrogels.

Synthetic hydrogels displaying cartilage-mimetic bulk and surface properties may serve as cartilage substitutes. Multi-network, electrostatic hydrogels that leverage intra- and inter-network repulsive and attractive forces represent a promising approach. Herein, triple network (TN) hydrogels were prepared to obtain a combination of desired characteristics (i.e., hydration, stiffness, shear stress, and friction properties). The TN hydrogels were comprised of a negatively charged 1st network and a neutral 2nd network possessing hydrophobic associations. Presumed to significantly influence surface properties, the 3rd network charge was systematically varied as cationic, anionic, and zwitterionic. A double-network (DN) hydrogel, comprised of the same 1st and 2nd network as for the TN hydrogels, was included as a control as well as native cartilage specimens. Micro-indentation was performed with a steel ball, yielding stiffness values as well as the contact area during sliding. The lubrication in both deionized (DI) water and fetal bovine serum (FBS) was evaluated with the micro-indenter wherein the stage reciprocated in a range of speeds. All the TN hydrogels exhibited greater Youngs modulus than the DN hydrogel control. The TN bearing a cationic 3rd network exhibited an exceptionally high Youngs modulus of ≈1.4 MPa, which was even higher than that of the cartilage samples. In both DI water and FBS, for most testing speeds, the TN hydrogels exhibited lower friction coefficient (COF) values and lower shear stresses than DN hydrogel as well as the native cartilage specimens.

A highly conductive and ultra-stretchable polyaniline/cellulose nanocrystal/polyacrylamide hydrogel with hydrophobic associations for wearable strain sensors

A highly stretchable hydrogel with extraordinary conductivity forms by polymerizing polyaniline within polyacrylamide. The latter contains hydrophobic associations and cellulose nanocrystals to provide excellent mechanical properties.

Interactions of Turmeric- and Curcumin-Functionalized Gold Nanoparticles with Human Serum Albumin: Exploration of Protein Corona Formation, Binding, Thermodynamics, and Antifibrillation Studies.

In order to better understand the bioavailability and biocompatibility of polyphenol-assisted surface-modified bioengineered nanoparticles in nanomedicine applications, here, we address a series of photophysical experiments to quantify the binding affinity of serum albumin toward polyphenol-capped gold nanoparticles. For this, two different gold nanoparticles (AuNPs) were synthesized via the green synthesis approach, where curcumin and turmeric extract act as reducing as well as capping agents. The size, surface charge, and surface plasmon bands of the AuNPs were highly affected by the adsorption of human serum albumin (HSA) during protein corona formation, which was investigated using dynamic light scattering (DLS), ξ-potential, ultraviolet-visible (UV-vis) spectroscopy, and transmission electron microscopy (TEM) measurements. Fluorescence-based methods, absorbance, and SERS experiments were carried out to evaluate the binding aspects of AuNPs with HSA. We found that the AuNPs show moderate binding affinity toward HSA (Kb ∼ 104 M-1), irrespective of the capping agents on the surface. Hydrophobic association, along with some contribution of electrostatic interaction, played a key role in the binding process. The binding interaction was more toward the subdomain IIA region of HSA, as indicated by the competitive displacement studies using site-specific binders (warfarin and flufenamic acid). Because of the large surface curvature of small-sized AuNPs, the secondary structural conformations of HSA were slightly altered, as revealed by circular dichroism (CD), Fourier transform infrared (FT-IR) spectroscopy, and surface-enhanced Raman scattering (SERS) measurements. Additionally, the findings of the binding interactions were re-evaluated using molecular dynamics (MD) simulation studies by determining the root-mean-square deviation (RMSD), root-mean-square fluctuation (RMSF), radius of gyration (Rg), and changes in the binding energy of HSA upon complexation with AuNPs. To determine the tentative evidence for pharmacokinetic administration, these biocompatible AuNPs were applied to inhibit the amyloid fibril formation of HSA and monitored by using the thioflavin T (ThT) assay, ANS fluorescence assay, fluorescence microscopic imaging, and FESEM. AuNPs were found to show better resistance toward fibrillation of the adsorbed protein.

Development of temperature- and salt-resistant viscosifier with dual skeleton structure of microcrosslinking and hydrophobic association structures and its application in water-based drilling fluids

In the process of developing deep oil and gas resources, the problem of high temperature and high salinity in deep strata has become a serious challenge faced by water-based drilling fluids. Under high temperature and high salinity conditions, drilling fluids must maintain good rheological properties to ensure safe and efficient drilling work. In this study, a temperature- and salt-resistant viscosifier (DASL) was synthesized using N, N-dimethylacrylamide, 2-Acrylamido-2-methylpropane sulfonic acid, sodium p-styrene sulfonate, and lauryl methacrylate as monomers with a double backbone structure of micro crosslinking and hydrophobic association structures. The results of pyrene fluorescence probe test and transmission electron microscopy observation showed that DASL has an obvious hydrophobic associative structure. Moreover, due to the presence of microcrosslinked structure, DASL exhibits good shear thinning property and thixotropy in aqueous solution. Under the conditions of 200 ℃ and 35 wt% NaCl, the apparent viscosity of the drilling fluid with 2 wt% DASL added was 24.5 mPa⸱s, and the filtration was only 9.2 mL. In addition, mechanism studies have shown that the dual skeleton structure of DASL improves its temperature and salt resistance. DASL can adsorb and bridge with bentonite particles, increase the internal friction and structural viscosity of the drilling fluid, enhance the internal mesh structure of the drilling fluid, improve the colloidal stability of the drilling fluid, and maintain a reasonable particle size distribution of the bentonite particles, which enable DASL to significantly increase the viscosity of the drilling fluid while reducing the filtration loss of the drilling fluid. This work demonstrates that polymers with dual skeleton structures of micro crosslinking and hydrophobic association have good application effects as temperature- and salt-resistant viscosifier for water-based drilling fluids.

Thermoresponsive Alginate-Graft-pNIPAM/Methyl Cellulose 3D-Printed Scaffolds Promote Osteogenesis In Vitro.

In this work, a sodium alginate-based copolymer grafted by thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) chains was used as gelator (Alg-g-PNIPAM) in combination with methylcellulose (MC). It was found that the mechanical properties of the resulting gel could be enhanced by the addition of MC and calcium ions (Ca2+). The proposed network is formed via a dual crosslinking mechanism including ionic interactions among Ca2+ and carboxyl groups and secondary hydrophobic associations of PNIPAM chains. MC was found to further reinforce the dynamic moduli of the resulting gels (i.e., a storage modulus of ca. 1500 Pa at physiological body and post-printing temperature), rendering them suitable for 3D printing in biomedical applications. The polymer networks were stable and retained their printed fidelity with minimum erosion as low as 6% for up to seven days. Furthermore, adhered pre-osteoblastic cells on Alg-g-PNIPAM/MC printed scaffolds presented 80% viability compared to tissue culture polystyrene control, and more importantly, they promoted the osteogenic potential, as indicated by the increased alkaline phosphatase activity, calcium, and collagen production relative to the Alg-g-PNIPAM control scaffolds. Specifically, ALP activity and collagen secreted by cells were significantly enhanced in Alg-g-PNIPAM/MC scaffolds compared to the Alg-g-PNIPAM counterparts, demonstrating their potential in bone tissue engineering.

Reversible, ultra-strong underwater adhesive based on supramolecular interaction for instant liquid leakage sealing and robust tissue adhesion

Underwater adhesives have great potential applications in biomedical fields. However, it is challenging to realize underwater adhesion due to screening by highly hydrated layer at the interface. To tackle this problem, here we present a novel strategy that combines hydrophobic association and supramolecular interactions to achieve robust adhesion at wet interfaces. Hydrophobic monomers (hexyl acrylate and styrene) are copolymerized with hydrophilic acrylic acid (AAc), and bifunctional host/guest assembly of β-cyclodextrin and adamantane to produce an adhesive. Herein, hydrophobic segments segregate to form hydrophobic microdomains both inside and at the interface. Internal hydrophobic clusters and host–guest interactions serve as physical crosslinks to improve the mechanical properties. Meanwhile, hydrophobic domains at surface play a critical role in expelling water and building a hydrophobic environment to minimize interference from water, where the hydrophilic units form hydrogen bonding, electrostatic attraction, coordination, and cation-π interactions to adhere on the surface. Lap shear tests indicate adhesion strength of about 92 ∼ 116 kPa on glass, copper, plastic, wood, and bone. Such a strong adhesion is independent of environment changes, including pH, PBS and NaCl solutions. More importantly, the adhesive shows excellent adhesion performance for bone, with adhesion strength up to 112.58 kPa in air and 91.51 kPa underwater. The strategy to combine hydrophobic interactions and supramolecular interactions may open a new avenue to the development of new adhesives for underwater adhesion and biological tissue.

Synergistic mechanism of dodecylamine/octanol mixtures enhancing lepidolite flotation from the self-aggregation behaviors at the air/liquid interface

Surface tension measurements and molecular dynamics (MD) simulations were used to explore the flotation foam properties and self-aggregation behaviors of dodecylamine (DDA)/octanol (OCT) mixtures formed with different mole ratios at the air/liquid interface. Based on the surface and thermodynamic parameters, the DDA/OCT mixtures exhibited greater interfacial activities and adsorption capacities than their individual components. The MD simulations showed that DDA and OCT were aggregated through hydrogen bonding, coulombic forces and hydrophobic association. OCT was inserted into the DDA adsorption layer, causing the alkyl chains of both DDA and OCT to extend from water to air at varying heights and angles. The addition of OCT improved the hydration of the amino groups and reduced the overall number of hydrogen bonds. The stability of the flotation foam decreased, and the high viscosity and difficult defoaming of the DDA flotation foam were significantly improved. When the DDA/OCT mole ratio was 2:1, the included angle formed between the alkyl chains and the interface was maximized, leading to enhanced compatibility among the alkyl chains, and the hydrogen bond energy was relatively large, which showed a strong synergistic effect. The MD simulation findings were consistent with the results obtained from the lepidolite flotation and surface tension experiments conducted in this study; our results could provide a theoretical foundation for the selection of superior mixed collectors and frothers.

Synthesis and properties of self‐healing hydrogel plugging agent

AbstractThe P(AM‐co‐AMPS)/SA DN hydrogel was synthesized through aqueous polymerization in this study. It formed a crosslinking network with hydrophobic associations between acrylamide (AM) and lauryl methacrylate (LMA), as well as an ionic bond network involving sodium alginate and Ca2+. To enhance its high‐temperature resistance, 2‐acrylamide‐2‐methylpropane sulfonic acid (AMPS) was incorporated into the hydrogel formulation. The structure of the hydrogel was characterized using Fourier transform infrared spectrometer (FTIR), thermogravimetric analyzer (TGA), and scanning electron microscopy (SEM) techniques. Results demonstrated that the hydrogel exhibited excellent temperature resistance and possessed a porous structure. Mechanical testing revealed a high tensile strength of 110 kPa, elongation at break of 995.31%, along with good fatigue resistance and self‐recovery performance during multiple cyclic stretching. Healing experiments indicated that the healing strength of the hydrogel was influenced by temperature variations. Furthermore, pressure plugging tests were conducted on steel models with crack widths of 0.5 and 1 mm, respectively; it was found that the 0.8%P(AM‐co‐AMPS)/SA DN hydrogel could withstand pressures up to 4.5 MPa at a temperature of 70°C. This novel hydrogel material exhibits remarkable mechanical properties along with certain self‐healing capabilities, making it suitable for leak control applications.

Hydrophobically Associated Hydrogel for High Sensitivity and Resolution of an Interdigital Electrode Pressure Sensor.

Hydrogel-based flexible strain sensors have been known for their excellent ability to convert different motions of humans into electrical signals, thus enabling real-time monitoring of various human health parameters. In this work, a composite hydrogel with hydrophobic association and hybrid cross-linking was fabricated by using polyacrylamide (PAm), surfactant sodium dodecyl sulfate (SDS), lauryl methacrylate (LMA), and polypyrrole (PPy). The dynamic dissociation-conjugation among LMA, SDS, and PPy could dissipate energy to improve the toughness of hydrogels. The SDS/PPy/LMPAm composite hydrogel with a toughness of 1.44 MJ/m3, tensile fracture stress of 345 kPa, tensile strain of 1021%, and electrical conductivity of 0.57 S/m was obtained. Furthermore, an interdigital electrode flexible pressure sensor was designed to replace the bipolar electrode flexible pressure sensor, which greatly improved the sensitivity and resolution of the pressure sensor. The SDS/PPy/LMPAm composite hydrogel-based interdigital electrode flexible pressure sensor showed extraordinary stability and identified different hand gestures as well as monitored the pulse signal of humans. Moreover, the characteristic systolic and diastolic peaks were clearly observed. The pulse frequency (65 times/min) and the radial artery augmentation index (0.57) were calculated, which are very important in evaluating the arterial vessel wall and function of human arteries.

Molecularly designed nonionic hydrophobic association polymers with anti-salt capacity: Enhancing drag reduction at high mineralization levels

The development of advanced anti-salt drag reduction (DR) agents is crucial for enhancing oil recovery rates, particularly in highly mineralized saline water where the network structure of polymers is prone to disruption, resulting in decreased DR. To address this problem, by carefully designing the structure of the hydrophobic association polymer, a new hydrophobic monomer called APO-10 was introduced, which successfully integrated water-soluble groups, and greatly enhanced the polymer's association properties in an aqueous solution. This ingenious approach produced a stable and robust network structure that can effectively resist the harmful effects of salt ions. PAPO-10 was synthesized through free radical polymerization and has hydrophilic EO chains that enhance its water solubility, enabling better extension of the hydrophobic long chain on the tail in solution. This facilitates the association between molecular chains, leading to the formation of a stable network structure even at low concentrations. PAPO-10 demonstrates remarkable properties, including rapid dissolution and exceptional resistance to salt. It delivers a remarkable DR of up to 78.2466 % at a concentration of 500 mg/L, dissolving within a mere 2 min in aqueous solutions. Molecular dynamics simulations confirmed that PAPO-10 exhibits strong polymer chain binding in solution, consistent with experimental results. Overall, this study provides valuable insights into the development of anti-salt polymers in slick fracturing.

Coagulation of Hydrophobic Ionic Associates of Cetyltrimethylammonium Bromide and Carrageenan.

In aqueous solutions, cetyltrimethylammonium cations bind to carrageenan polyanions, and the resulting ionic associates form macroscopic aggregates due to hydrophobic interaction. At certain ratios of cetyltrimethylammonium to carrageenan, the resulting colloidal particles auto-flocculate. According to visual observations, the ratio ranges from 1 to 3 mmol/g; otherwise the suspensions are stable. By measuring the sedimentation rate and particle size distribution, the most extensive flocculation was found to be from 1.7 to 2.3 mmol/g. The ratio corresponding to the fastest auto-flocculation was precisely determined by titrating the reagents with small increments and recording the turbidity. The turbidimetric titration plots contain distinct break points corresponding to the most extensive flocculation. These break points occur at the same ratio of carrageenan to cetyltrimethylammonium over a wide range of reagent concentrations. The precise values of the critical ratio were found to be 1.78 and 1.53 mmol/g, respectively, during the titration of cetyltrimethylammonium with carrageenan and vice versa. The number of anionic sulfate groups in carrageenan was measured by ICP OES and found to be 1.35 mmol/g. This value is consistent with the critical ratio of the auto-flocculation.

Polymerization Behavior and Rheological Properties of a Surfactant-Modified Reactive Hydrophobic Monomer

The structures and properties of hydrophobic association polymers can be controlled using micelles. In this work, we synthesize a reactive hydrophobic surfactant monomer, KS-3, from oleic acid, N,N-dimethylpropylenediamine, and allyl chloride. A strong synergistic effect between KS-3 and cocamidopropyl betaine in aqueous solution enhances the hydrophilic dispersibility of KS-3, thereby transforming spherical micelles into cylindrical micelles. KS-3 was grafted onto a polyacrylamide chain via aqueous free-radical polymerization to obtain RES, a hydrophobic association polymer. Structural analysis revealed that the RES polymers assembled in wormlike micelles were more tightly arranged than those assembled in spherical micelles, resulting in a compact network structure in water, smooth surface, and high thermal stability. Rheological tests revealed that the synthesized polymers with wormlike and spherical micelles exhibited shear-thinning properties along with different structural strengths and viscoelasticities. Therefore, controlling the micellar state can effectively regulate the polymer properties. The polymers obtained through wormlike micelle polymerization have potential applications in fields with high demands, such as drug release, water purification, and oilfield development.

Triple physical cross-linking cellulose nanofibers-based poly(ionic liquid) hydrogel as wearable multifunctional sensors

A novel triple physical cross-linking poly(ionic liquid) hydrogel, composed of poly(acrylamide-co-dodecyl methacrylate-co-1-vinyl-3-methyluracil-imidazolium chloride)/cellulose nanofibers-Ca2+ (PADV/CNFs-Ca2+), was synthesized through micellar-copolymerization followed by a solvent-soaked procedure. The synergistic interactions in polymer network (i.e. the hydrophobic association of dodecyl methacrylate moiety in surfactant micelles, the hydrogen bondings between imidazolium monomer segments and other monomer segments in polymers, and the ionic coordination between Ca2+ and -COO− on cellulose nanofibers surface) endowed the hydrogel with excellent mechanical properties, including high strength (754 kPa of tensile strength and 1905 kPa of compressive strength), outstanding stretchability (1963 %), elastic modulus (56.5 kPa) and remarkable mechanical durability (200 cycles with 500 % deformations and 100 cycles at 50 % compression strain). Besides, this hydrogel exhibited other advantages, such as satisfied conductivity (28.7 mS/cm), high strain/pressure/temperature-sensitive behavior, precise and stable signal transmission, varying degrees of antibacterial activity, and biocompatibility. Owing to the exceptional comprehensive performance, the hydrogel was then assembled as a multifunctional sensor to monitor the joint motion, vocal cord vibration, tactile sensation and body temperature with remarkable sensitivity in real time. This work offered a new strategy for the fabrication of durable, biocompatible, antibacterial and conductive materials for wearable multifunctional electronic devices.

High-Saline-Enabled Hydrophobic Homogeneous Cross-Linking for Extremely Soft, Tough, and Stretchable Conductive Hydrogels as High-Sensitive Strain Sensors.

Design of admirable conductive hydrogels combining robust toughness, soft flexibility, desirable conductivity, and freezing resistance remains daunting challenges for meeting the customized and critical demands of flexible and wearable electronics. Herein, a promising and facile strategy to prepare hydrogels tailored to these anticipated demands is proposed, which is prepared in one step by homogeneous cross-linking of acrylamide using hydrophobic divinylbenzene stabilized by micelles under saturated high-saline solutions. The influence of high-saline environments on the hydrogel topology and mechanical performance is investigated. The high-saline environments suppress the size of hydrophobic cross-linkers in micelles during hydrogel polymerization, which weaken the dynamic hydrophobic associations to soften the hydrogels. Nevertheless, the homogeneous cross-linked networks ensure antifracture during ultralarge deformations. The obtained hydrogels show special mechanical performance combining extremely soft deformability and antifracture features (Young's modulus, 5 kPa; stretchability, 10200%; toughness, 134 kJ m-2; and excellent anticrack propagation). The saturated-saline environments also endow the hydrogels with desirable ion conductivity (106 mS cm-1) and freezing resistance (<20 °C). These comprehensive properties of the obtained hydrogels are quite suitable for flexible electronic applications, which is demonstrated by the high sensitivity and durability of the derived strain sensors.