2-hydroxyethyl Acrylamide Research Articles

Antimicrobial Peptide SAAP‐148‐Functionalized Hydrogels from Photocrosslinkable Polymers with Broad Antibacterial Activity

AbstractAntimicrobial peptides (AMPs) are promising alternatives to traditional antibiotics for treating skin wound infections. Nonetheless, their short half‐life in biological environments restricts clinical applicability. Covalent immobilization of AMPs onto suitable substrates offers a comprehensive solution, creating contact‐killing surfaces with long‐term functionality. Here, a copolymer of poly[(hydroxy ethyl acrylamide)‐co‐(4‐benzophenone acrylamide)‐co‐(pentafluorophenyl acrylate)‐co‐(ECOSURF EH‐3 acrylate)], in short poly(HEAAm‐co‐BPAAm‐co‐PFPA‐co‐EH3A), is synthesized by free radical polymerization. Subsequent modification of active ester groups with the amine groups of SAAP‐148, results in a copolymer, that is non‐cytotoxic to human lung fibroblasts. UV photocrosslinking of the benzophenone units yields a polymer network that forms a hydrogel after swelling with aqueous medium. Both the SAAP‐148‐modified polymer in solution and the photocrosslinked hydrogels show good antimicrobial activity against strains of Escherichia coli, Staphylococcus aureus, Pseudomonas aeruginosa, and Acinetobacter baumannii, including multidrug‐resistant strains, frequently found in wound infections. The covalent attachment of SAAP‐148 prevents leaching, ensuring sustained antimicrobial activity for at least 48 h in diluted human blood plasma and 14 days in PBS. This prolonged retention of antimicrobial activity in human blood plasma significantly enhances its clinical potential. Overall, this study shows the potential of the AMP‐functionalized photocrosslinkable polymer as antimicrobial wound dressings, providing an effective alternative to antibiotics.

Fully Physically Crosslinked Hydrogel with Ultrastretchability, Transparency, and Freezing-Tolerant Properties for Strain Sensor.

Nowadays, conductive hydrogels show significant prospects as strain sensors due to their good stretchability and signal transduction abilities. However, traditional hydrogels possess poor anti-freezing performance at low temperatures owing to the large number of water molecules, which limits their application scope. To date, constructing a hydrogel-based sensor with balanced stretchability, conductivity, transparency, and anti-freezing properties via simple methods has proven challenging. Here, a fully physically crosslinked poly(hydroxyethyl acrylamide)-glycerol-sodium chloride (PHEAA-Gl-NaCl) hydrogel was obtained by polymerizing hydroxyethyl acrylamide in deionized water and then soaking it in a saturated NaCl solution of glycerol and water. The PHEAA-Gl-NaCl hydrogel had good transparency (~93%), stretchability (~1300%), and fracture stress (~287 kPa). Owing to the presence of glycerol and sodium chloride, the PHEAA-Gl-NaCl hydrogel had good anti-freezing properties and conductivity. Furthermore, the PHEAA-Gl-NaCl hydrogel-based strain sensor possessed good sensitivity and cyclic stability, enabling the detection of different human motions stably and in a wide temperature range. Based on the above characteristics, the PHEAA-Gl-NaCl hydrogel has broad application prospects in flexible electronic materials.

A novel poly(2-hydroxyethyl acrylamide) copolymer for the fabrication of transparent antifogging coatings on polycarbonate substrates

Although polycarbonate (PC) is widely used in various applications, its inherent hydrophobicity limits its potential in applications that require high light transmittance due to surface fog caused by changes in temperature or humidity in the environment. This work presents a facile method to fabricate transparent antifogging coatings on PC substrates based on poly(2-hydroxyethyl acrylamide-co-2-aminoethyl methacrylate) (P(HEAA-co-AEMA)), in which the AEMA segments have an amino functional group that can react with the ester group on the surface of the PC substrate to form covalent urethane bonds during the heat curing process, avoiding the problems of coating susceptibility to mechanical damage, ease of peeling, etc. Moreover, HEAA units are employed as hydrophilic groups, providing antifogging performance. These antifogging coatings can be easily obtained by coating P(HEAA-co-AEMA) copolymers on PC substrates at room temperature and then curing them by thermal treatment. These transparent coatings exhibited excellent antifogging and self-cleaning performance. Furthermore, the coatings exhibited good adhesion in the cross-cut test and thermal stability in the hot water resistance test. Therefore, the present P(HEAA-co-AEMA) copolymer coatings are promising for practical antifogging applications.

Low-Viscosity Route to High-Molecular-Weight Water-Soluble Polymers: Exploiting the Salt Sensitivity of Poly(N-acryloylmorpholine).

We report a new one-pot low-viscosity synthetic route to high molecular weight non-ionic water-soluble polymers based on polymerization-induced self-assembly (PISA). The RAFT aqueous dispersion polymerization of N-acryloylmorpholine (NAM) is conducted at 30 °C using a suitable redox initiator and a poly(2-hydroxyethyl acrylamide) (PHEAC) precursor in the presence of 0.60 M ammonium sulfate. This relatively low level of added electrolyte is sufficient to salt out the PNAM block, while steric stabilization is conferred by the relatively short salt-tolerant PHEAC block. A mean degree of polymerization (DP) of up to 6000 was targeted for the PNAM block, and high NAM conversions (>96%) were obtained in all cases. On dilution with deionized water, the as-synthesized sterically stabilized particles undergo dissociation to afford molecularly dissolved chains, as judged by dynamic light scattering and 1H NMR spectroscopy studies. DMF GPC analysis confirmed a high chain extension efficiency for the PHEAC precursor, but relatively broad molecular weight distributions were observed for the PHEAC-PNAM diblock copolymer chains (Mw/Mn > 1.9). This has been observed for many other PISA formulations when targeting high core-forming block DPs and is tentatively attributed to chain transfer to polymer, which is well known for polyacrylamide-based polymers. In fact, relatively high dispersities are actually desirable if such copolymers are to be used as viscosity modifiers because solution viscosity correlates closely with Mw. Static light scattering studies were also conducted, with a Zimm plot indicating an absolute Mw of approximately 2.5 × 106 g mol-1 when targeting a PNAM DP of 6000. Finally, it is emphasized that targeting such high DPs leads to a sulfur content for this latter formulation of just 23 ppm, which minimizes the cost, color, and malodor associated with the organosulfur RAFT agent.

Enhancing Robustness of Adhesive Hydrogels through PEG-NHS Incorporation.

Tissue wounds are a significant challenge for the healthcare system, affecting millions globally. Current methods like suturing and stapling have limitations as they inadequately cover the wound, fail to prevent fluid leakage, and increase the risk of infection. Effective solutions for diverse wound conditions are still lacking. Adhesive hydrogels, on the other hand, can be a potential alternative for wound care. They offer benefits such as firm sealing without leakage, easy and rapid application, and the provision of mechanical support and flexibility. However, the in vivo durability of hydrogels is often compromised by excessive swelling and unforeseen degradation, which limits their widespread use. In this study, we addressed the durability issues of the adhesive hydrogels by incorporating acrylamide polyethylene glycol N-hydroxysuccinimide (PEG-NHS) moieties (max. 2 wt %) into hydrogels based on hydroxy ethyl acrylamide (HEAam). The results showed that the addition of PEG-NHS significantly enhanced the adhesion performance, achieving up to 2-fold improvement on various soft tissues including skin, trachea, heart, lung, liver, and kidney. We further observed that the addition of PEG-NHS into the adhesive hydrogel network improved their intrinsic mechanical properties. The tensile modulus of these hydrogels increased up to 5-fold, while the swelling ratio decreased up to 2-fold in various media. These hydrogels also exhibited improved durability under the enzymatic and oxidative biodegradation induced conditions without causing any toxicity to the cells. To evaluate its potential for clinical applications, we used PEG-NHS based hydrogels to address tracheomalacia, a condition characterized by inadequate mechanical support of the airway due to weak/malacic cartilage rings. Ex vivo study confirmed that the addition of PEG-NHS to the hydrogel network prevented approximately 90% of airway collapse compared to the case without PEG-NHS. Overall, this study offers a promising approach to enhance the durability of adhesive hydrogels by the addition of PEG-NHS, thereby improving their overall performances for various biomedical applications.

Effect of varying functional monomers in experimental self-adhesive composites: polymerization kinetics, cell metabolism influence and sealing ability

The aim was to evaluate the effects of adding different functional monomers to experimental self-adhesive composites (SACs) on polymerization kinetics, cell metabolic activity, and sealing ability. SACs were formulated using urethane dimethacrylate as the base monomer and triethylene glycol dimethacrylate. Additionally, 10 wt.% of distinct functional monomers were added - 10-methacryloyloxydecyl dihydrogen phosphate, glycerol phosphate dimethacrylate (GPDM), 2-hydroxyethyl methacrylate (HEMA) or hydroxyethyl acrylamide (HEAA). ATR-FTIR was used to determine real-time polymerization kinetics (20 min, n = 3). The final extrapolated conversion and polymerization rates were determined (DC ,max; Rp ,max). The DC ,max values were employed to calculate volumetric shrinkage. The MTT assay was performed on MDPC-23 cells using disc extracts at different concentrations (n = 8). Class V cavities were prepared in 60 sound human molars, assigned to six groups (n = 10), depending on the composite used and aging type (T0 or TC, if thermocycled for 10 000 cycles). One-way ANOVA, two-way, and Kruskal–Wallis tests were employed to treat the data (ɑ = 0.05). Varying the functional monomers had a large impact on DC,max, as confirmed by one-way ANOVA (p<0.001). The highest was obtained for HEMA (64 ± 3%). The HEMA and HEAA formulations were found to be significantly more toxic at concentrations below 100%. For microleakage, having a functional monomer or not did not show any improvement, irrespective of margin or aging period (Mann–Whitney U, p > 0.05). Larger functional monomers MDP and GPDM affected polymerization properties. Conversely, their acidity did not seem to be detrimental to cell metabolic activity. Regarding sealing ability, it seems that the functional monomers did not bring an advantage to the composites. Varying the functional monomer in SACs had a clear impact on the polymerization kinetics as well as on their cytotoxic potential. However, it did not confer better microleakage and sealing. Claiming self-adhesiveness based only on functional monomers seems dubious.

Fully Physically Crosslinked Conductive Hydrogel with Ultrastretchability, Transparency, and Self-Healing Properties for Strain Sensors.

Currently, conductive hydrogels have received great attention as flexible strain sensors. However, the preparation of such sensors with integrated stretchability, transparency, and self-healing properties into one gel through a simple method still remains a huge challenge. Here, a fully physically crosslinked double network hydrogel was developed based on poly(hydroxyethyl acrylamide) (PHEAA) and κ-carrageenan (Car). The driving forces for physical gelation were hydrogen bonds, ion bonding, and electrostatic interactions. The resultant PHEAA-Car hydrogel displayed stretchability (1145%) and optical transparency (92%). Meanwhile, the PHEAA-Car hydrogel exhibited a self-healing property at 25 °C. Additionally, the PHEAA-Car hydrogel-based strain sensor could monitor different joint movements. Based on the above functions, the PHEAA-Car hydrogel can be applied in flexible strain sensors.

New Formulation of Platelet-Rich Plasma Enriched in Platelet and Extraplatelet Biomolecules Using Hydrogels.

Platelet-rich plasma (PRP) is an autologous biologic product used in several fields of medicine for tissue repair due to the regenerative capacity of the biomolecules of its formulation. PRP consists of a plasma with a platelet concentration higher than basal levels but with basal levels of any biomolecules present out of the platelets. Plasma contains extraplatelet biomolecules known to enhance its regenerative properties. Therefore, a PRP containing not only a higher concentration of platelets but also a higher concentration of extraplatelet biomolecules that could have a stronger regenerative performance than a standard PRP. Considering this, the aim of this work is to develop a new method to obtain PRP enriched in both platelet and extraplatelet molecules. The method is based on the absorption of the water of the plasma using hydroxyethyl acrylamide (HEAA)-based hydrogels. A plasma fraction obtained from blood, containing the basal levels of platelets and proteins, was placed in contact with the HEAA hydrogel powder to absorb half the volume of the water. The resulting plasma was characterized, and its bioactivity was analyzed in vitro. The novel PRP (nPRP) showed a platelet concentration and platelet derived growth factor (PDGF) levels similar to the standard PRP (sPRP), but the concentration of the extraplatelet growth factors IGF-1 (p < 0.0001) and HGF (p < 0.001) were significantly increased. Additionally, the cells exposed to the nPRP showed increased cell viability than those exposed to a sPRP in human dermal fibroblasts (p < 0.001) and primary chondrocytes (p < 0.01). In conclusion, this novel absorption-based method produces a PRP with novel characteristics compared to the standard PRPs, with promising in vitro results that could potentially trigger improved tissue regeneration capacity.

Wet adhesive hydrogels to correct malacic trachea (tracheomalacia) A proof of concept

Tracheomalacia (TM) is a condition characterized by a weak tracheal cartilage and/or muscle, resulting in excessive collapse of the airway in the newborns. Current treatments including tracheal reconstruction, tracheoplasty, endo- and extra-luminal stents have limitations. To address these limitations, this work proposes a new strategy by wrapping an adhesive hydrogel patch around a malacic trachea. Through a numerical model, first it was demonstrated that a hydrogel patch with sufficient mechanical and adhesion strength can preserve the trachea's physiological shape. Accordingly, a new hydrogel providing robust adhesionon wet tracheal surfaces was synthesized employing the hydroxyethyl acrylamide (HEAam) and polyethylene glycol methacrylate (PEGDMA) as main polymer network and crosslinker, respectively. Exvivo experiments revealed that the adhesive hydrogel patches can restrain the collapsing of malacic trachea under negative pressure. This study may open the possibility of using an adhesive hydrogel as a new approach in the difficult clinical situation of tracheomalacia.

Stretchable Organohydrogel with Adhesion, Self-Healing, and Environment-Tolerance for Wearable Strain Sensors.

Stretchable hydrogels as landmark soft materials have been efficiently utilized in the field of wearable sensing devices. However, these soft hydrogels mostly cannot integrate transparency, stretchability, adhesiveness, self-healing, and environmental adaptability into one system. Herein, a fully physically cross-linked poly(hydroxyethyl acrylamide)-gelatin dual-network organohydrogel is prepared in a phytic acid-glycerol binary solvent via a rapid ultraviolet light initiation. The introduction of gelatin as the second network endows the organohydrogel with desirable mechanical performance (high stretchability up to 1240%). The presence of phytic acid not only synergizes with glycerol to impart environment-tolerance to the organohydrogel (from -20 to 60 °C) but also increases the conductivity. Moreover, the organohydrogel demonstrates a durable adhesive performance toward diverse substrates, a high self-healing efficiency through heat treatment, and favorable optical transparency (transmittance of 90%). Furthermore, the organohydrogel achieves high sensitivity (gauge factor of 2.18 at 100% strain) and rapid response time (80 ms) and could detect both tiny (a low detection limit of 0.25% strain) and large deformations. Therefore, the assembled organohydrogel-based wearable sensors are capable of monitoring human joint motions, facial expression, and voice signals. This work proposes a facile route for multifunctional organohydrogel transducers and promises the practical application of flexible wearable electronics in complex scenarios.

Acrylamide monomers in universal adhesives.

The mono-functional monomer 2-hydroxyethyl methacrylate (HEMA) is often added to universal adhesives (UAs) to improve surface wetting and prevent phase separation. Nevertheless, HEMA promotes water sorption and hydrolysis at adhesive interfaces, hereby affecting long-term bonding to dentin. This study investigated if two acrylamide monomers could replace HEMA in an UA formulation applied in etch-and-rinse (2E&R) and self-etch (1SE) bonding mode. Four experimental UAs were bonded to bur-cut dentin. In addition to 12wt% 10-MDP, 25wt% Bis-GMA and 10wt% TEGDMA as common monomer composition, 20 %wt ethanol and 15 %wt water as solvent, and 3wt% polymerization-related additives, the four formulations solely differed for either the acrylamide cross-linker monomer 'FAM-201' as TEGDMA alternative and HEMA replacement, the hydroxyethyl acrylamide monomer 'HEAA' as HEMA alternative, HEMA ('HEMA+'), or extra TEGDMA in a HEMA-free control ('HEMA-'), all added in a 15wt% concentration. The split-tooth study design involved application in 2E&R mode on one tooth half versus 1SE mode on the corresponding half. Micro-tensile bond strength of half of the micro-specimens was measured upon 1-week distilled water storage ('immediate' 1w μTBS), with the other half measured after additional 6-month storage ('aged' 6m μTBS). Statistics involved linear mixed-effects (LME) modelling (p<.05). Additionally, interfacial TEM characterization, thin-film (TF) XRD surface analysis, LogP determination, and a cytotoxicity assay were carried out. FAM-201 revealed significantly higher μTBS than HEMA+at 1w and 6m when applied both in E&R and SE bonding modes. HEAA's μTBS was significantly lower than that of HEMA+at 1w when applied in SE mode. TF-XRD and TEM revealed similar chemical and ultrastructural interfacial characterization, including stable 10-MDP_Ca salt nano-layering. FAM-201 was least cytotoxic and presented with an intermediary LogP, while HEAA presented with the highest LogP, indicating high hydrophilicity and water-sorption sensitivity. The acrylamide co-monomer FAM-201 could replace HEMA in an UA formulation, while HEAA not.

Fully physically crosslinked organohydrogel with ultrastretchability, transparency, freezing-tolerant, self-healing, and adhesion properties for strain sensor

Recently, conductive hydrogels have gained great attention in intelligent wearable devices, but the simultaneous realization of stretchability, transparency, anti-freezing, self-healing, and adhesion properties by an easy method is still a big challenge. Herein, a novel multifunctional organohydrogel based on noncovalent intermolecular interactions was developed by simply polymerization hydroxyethyl acrylamide (HEAA) in LiCl cryoprotectant/water (Cryo/water) solution via one-pot photo-polymerization method. Hydrogen bonding interactions of PHEAA-PHEAA and PHEAA-Cryo were the main driving force for gel formation. The LiCl and cryoprotectant gave PHEAA-Cryo-LiCl organohydrogel good conductivity and anti-freezing properties, respectively. The effects of the gel composition on the mechanical, transparency, anti-freezing, and conductivity properties of PHEAA-Cryo-LiCl organohydrogels were researched in detail. Moreover, poly(hydroxyethyl acrylamide)-glycerin-lithium chloride (PHEAA-Gl-LiCl) organohydrogel displayed good self-healing and adhesion properties owing to the reversible hydrogen bonding. Based on PHEAA-Gl-LiCl organohydrogel, a strain sensor was prepared for detecting human movements within a wide temperature range (−40 °C–25 °C), and the result showed various human motions could be detected stably, including joint movement, making a fist, swallowing or pronouncing, suggesting the potential application for the next generation of intelligent wearable sensors.

ABA block copolymers comprising a water soluble poly(N-hydroxyethyl acrylamide) B block form self-assemblies of varied morphologies in an aqueous environment

ABA block copolymers synthesized by a combination of SET-LRP and photoinduced LRP techniques form self-assemblies of varied morphologies in an aqueous environment and show low cell toxicity.

Smart Antifreeze Hydrogels with Abundant Hydrogen Bonding for Conductive Flexible Sensors.

Recently, flexible sensors based on conductive hydrogels have been widely used in human health monitoring, human movement detection and soft robotics due to their excellent flexibility, high water content, good biocompatibility. However, traditional conductive hydrogels tend to freeze and lose their flexibility at low temperature, which greatly limits their application in a low temperature environment. Herein, according to the mechanism that multi−hydrogen bonds can inhibit ice crystal formation by forming hydrogen bonds with water molecules, we used butanediol (BD) and N−hydroxyethyl acrylamide (HEAA) monomer with a multi−hydrogen bond structure to construct LiCl/p(HEAA−co−BD) conductive hydrogel with antifreeze property. The results indicated that the prepared LiCl/p(HEAA−co−BD) conductive hydrogel showed excellent antifreeze property with a low freeze point of −85.6 °C. Therefore, even at −40 °C, the hydrogel can still stretch up to 400% with a tensile stress of ~450 KPa. Moreover, the hydrogel exhibited repeatable adhesion property (~30 KPa), which was attributed to the existence of multiple hydrogen bonds. Furthermore, a simple flexible sensor was fabricated by using LiCl/p(HEAA−co−BD) conductive hydrogel to detect compression and stretching responses. The sensor had excellent sensitivity and could monitor human body movement.

Nanofiber veil applied in toughness enhancement of thermoplastic carbon fiber composites

This study presents an experimental investigation on thermoplastic carbon fiber composite based on PMMA resin interleaved with Polyamide electrospun nanofiber veils. In particular, the effect of improving the interfacial adhesion of the resin to nanofiber and carbon fiber on the fracture behavior of the laminates and the corresponding fracture mechanism was studied by using different molar concentrations of functional monomer hydroxyethyl acrylamide (HEAA) for copolymerization with methyl methacrylate. The effectiveness of the nanoreinforce has been addressed by Mode-Ⅰ and Mode-Ⅱ tests. The results showed that the fracture toughness of Mode-Ⅰ decreased firstly and then increased with an increase in HEAA feed with 0–5 mol% due to the change of crack tip path accompanied by the bridging mechanism shifting, the best performance was founded in 5 mol% HEAA-copolymerized thermoplastic carbon fiber composites (CFRTP) samples (17.6% for initiation and 28% for propagation); whereas a characteristic of increasing firstly and then decreasing performed under Mode-Ⅱ loading due to the formation of multilayer microcrack in nano-toughing matrix layer, the 3 mol% HEAA-copolymerized CFRTP samples exhibited good improvement (137% for initiation and 147% for propagation).

Expanding the use of affordable CuSO4·5H2O in ATRP techniques in homogeneous media

Advances in atom transfer radical polymerization (ATRP) are usually focused on reducing the metal catalyst concentration, using low toxicity metals or even metal-free catalysts, to minimize or avoid the contamination of polymers. In this work, the less toxic and inexpensive CuSO4·5H2O was used to replace CuBr2, the most employed metal source for ATRP, to control polymerizations under homogeneous conditions. Well-defined (Đ ≤ 1.3) hydrophobic homopolymers of poly(methyl acrylate) (PMA), poly(methyl methacrylate) (PMMA), polystyrene (PS) and poly(butyl acrylate) (PBA) were obtained in various organic solvent/water mixtures with similar control as when CuBr2 was used. The main limitation is the lower solubility of the CuSO4/L complex in pure organic solvents compared with CuBr2/L. The preparation of several hydrophilic polymers, namely poly(2-hydroxyethyl acrylate) (PHEA), poly((3-acrylamidopropyl)trimethylammonium chloride) (PAMPTMA), poly(2-hydroxyethyl acrylamide) (PHEAA), polyacrylamide (PAAm), poly(N,N-dimethylacrylamide) (PDMAA), poly(2-aminoethyl methacrylate hydrochloride) (PAMA), poly[oligo(ethylene oxide) methyl ether acrylate] (POEOA) and biorelevant block copolymers (PHEA-b-PAMPTMA and PAMPTMA-b-PHEAA) was successfully carried out in aqueous medium using different ATRP techniques. Future studies on this system will include the use of CuSO4/L complexes in several organic solvents and in heterogeneous ATRP.

N-Hydroxyethyl acrylamide as a functional eROP initiator for the preparation of nanoparticles under "greener" reaction conditions.

N-Hydroxyethyl acrylamide was used as a functional initiator for the enzymatic ring-opening polymerisation of ε-caprolactone and δ-valerolactone. N-Hydroxyethyl acrylamide was found not to undergo self-reaction in the presence of Lipase B from Candida antarctica under the reaction conditions employed. By contrast, this is a major problem for 2-hydroxyethyl methacrylate and 2-hydroxyethyl acrylate which both show significant transesterification issues leading to unwanted branching and cross-linking. Surprisingly, N-hydroxyethyl acrylamide did not react fully during enzymatic ring-opening polymerisation. Computational docking studies helped us understand that the initiated polymer chains have a higher affinity for the enzyme active site than the initiator alone, leading to polymer propagation proceeding at a faster rate than polymer initiation leading to incomplete initiator consumption. Hydroxyl end group fidelity was confirmed by organocatalytic chain extension with lactide. N-Hydroxyethyl acrylamide initiated polycaprolactones were free-radical copolymerised with PEGMA to produce a small set of amphiphilic copolymers. The amphiphilic polymers were shown to self-assemble into nanoparticles, and to display low cytotoxicity in 2D in vitro experiments. To increase the green credentials of the synthetic strategies, all reactions were carried out in 2-methyl tetrahydrofuran, a solvent derived from renewable resources and an alternative for the more traditionally used fossil-based solvents tetrahydrofuran, dichloromethane, and toluene.

ABC-Type Triblock Copolyacrylamides via Copper-Mediated Reversible Deactivation Radical Polymerization.

The aqueous Cu(0)-mediated reversible deactivation radical polymerization (RDRP) of triblock copolymers with two block sequences at 0.0 °C is reported herein. Well-defined triblock copolymers initiated from PHEAA or PDMA, containing (A) 2-hydroxyethyl acrylamide (HEAA), (B) N-isopropylacrylamide (NIPAM) and (C) N, N-dimethylacrylamide (DMA), were synthesized. The ultrafast one-pot synthesis of sequence-controlled triblock copolymers via iterative sequential monomer addition after full conversion, without any purification steps throughout the monomer additions, was performed. The narrow dispersities of the triblock copolymers proved the high degree of end-group fidelity of the starting macroinitiator and the absence of any significant undesirable side reactions. Controlled chain length and extremely narrow molecular weight distributions (dispersity ~1.10) were achieved, and quantitative conversion was attained in as little as 52 min. The full disproportionation of CuBr in the presence of Me6TREN in water prior to both monomer and initiator addition was crucially exploited to produce a well-defined ABC-type triblock copolymer. In addition, the undesirable side reaction that could influence the living nature of the system was investigated. The ability to incorporate several functional monomers without affecting the living nature of the polymerization proves the versatility of this approach.

Facile Preparation of MXene/Poly(vinyl alcohol)/N-(2-Hydroxyethyl Acrylamide) Hydrogels with High Tensile Strength for Strain Sensors

In this paper, a novel conductive hydrogel was made by a one-pot method at 60 °C for 12 hours in one step without any cross-linking agent. The hydrogel was composited of Ti3C2 MXene nano slices, poly(vinyl alcohol) (PVA) and poly-N-(2-hydroxyethyl acrylamide) (PHEAA), named as MXene/PVA/PHEAA hydrogel. Compared with previous methods to make MXene hydrogel, this one-pot method was facile and fast. The as-prepared hydrogel was highly stretchable with the breaking elongation of 1300% and tensile strength of 1.1 MPa. MXene nano sheets dispersed in the hydrogel formed a three-dimensional conductive network, which increased the strength and conductivity of the gels. The conductivity changed with the gel’s deformation and could be applied as strain sensors. The strain sensors made of the hydrogels were highly stretchable, bendable and flexible with the response range of 1%–300% and a large gauge factor of 4.23. The sensors can be applied to detect human movements such as finger bending, leg bending, water drinking. The MXene/PVA/PHEAA hydrogel made by this facile one-pot method is promising to make strain sensors for health detection.

Ionic Conductive Organohydrogel With Ultrastretchability, Self-Healable and Freezing-Tolerant Properties for Wearable Strain Sensor

Currently, stretchable hydrogel has attracted great attention in the field of wearable flexible sensors. However, fabricating flexible hydrogel sensor simultaneously with superstretchability, high mechanical strength, remarkable self-healing ability, excellent anti-freezing and sensing features via a facile method remains a huge challenge. Herein, a fully physically linked poly(hydroxyethyl acrylamide)-gelatin-glycerol-lithium chloride (PHEAA-GE-Gl-LiCl) double network organohydrogel is prepared via a simple one-pot heating-cooling-photopolymerization method. The prepared PHEAA-GE-Gl-LiCl organohydrogel exhibits favorable stretchability (970%) and remarkable self-healing property. Meanwhile, due to the presence of glycerol and LiCl, the PHEAA-GE-Gl-LiCl organohydrogel possesses outstanding anti-freezing capability, it can maintain excellent stretchability (608%) and conductivity (0.102 S/m) even at −40°C. In addition, the PHEAA-GE-Gl-LiCl organohydrogel-based strain sensor is capable of repeatedly and stably detecting and monitoring both large-scale human motions and subtle physiological signals in a wide temperature range (from −40°C to 25°C). More importantly, the PHEAA-GE-Gl-LiCl organohydrogel-based sensor displays excellent strain sensitivity (GF = 13.16 at 500% strain), fast response time (300 ms), and outstanding repeatability. Based on these super characteristics, it is envisioned that PHEAA-GE-Gl-LiCl organohydrogel holds promising potentials as wearable strain sensor.