Robust hydrogel of regenerated cellulose by chemical crosslinking coupled with polyacrylamide network

Regenerated cellulose/polyacrylamide (RC/PAAm) double network (DN) hydrogels are composed of cellulose crosslinked by epichlorohydrin (ECH) and chemical-crosslinked PAAm. The prepared RC/PAAm DN hydrogels present enhanced strength, good shape recovery property, excellent energy dissipation properties, decreased equilibrium water content, and low equilibrium swelling ratio (SR). The compressive strength and modulus of RC/PAAm hydrogel are about 4.3 and 11.5 times compared to that of RC hydrogel, respectively. Intriguingly, the chemical crosslinking between ECH and cellulose chains could increase the distance between cellulose chains. Consequently, the increasing molar ratio of ECH to glucose leads to larger SRs and decreased mechanical strength of the hydrogels. Additionally, higher PAAm contents lead to more densely crosslinked networks, and thus decreasing the SRs and improving the mechanical strength of the hydrogels. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 47811.     

Mechanical Strengths of Hydrogels of Poly(N,N‐Dimethylacrylamide)/Alginate with IPN and of Poly(N,N‐Dimethylacrylamide)/Chitosan with Semi‐IPN Microstructures

Tough hydrogels receive continuous attention because of their promising applications in many fields. Herein, tough hydrogels of poly (N,N‐dimethylacrylamide) (PDMAA)/alginate (SA) are prepared, with interpenetrating network (IPN) and of PDMAA/chitosan (CS) with semi‐IPN microstructure, respectively. The toughening of the hydrogel by incorporating natural polymers is studied by compressing tests and dynamic mechanical analyses. Moreover, cyclic load–unload compressing of the two types of hydrogels are performed at low strains and under relatively high strains, in order to compare their strength and anti‐fatigue properties. The results indicate that the mechanical strength can be markedly improved upon addition of the natural polymers, and the IPN hydrogel of PDMAA/SA reveals much higher mechanical performances but is less stable. However, the semi‐IPN hydrogel of PDMAA/CS displays excellent anti‐fatigue stability, but with relatively low strength. Swelling tests, scanning electron microscopy, and Fourier transform infrared spectroscopy are carried out to study the microstructures of the hydrogels, which are carefully analyzed to understand the difference in mechanical performances of those hydrogels. The results suggest that the presence of sacrificial unit and higher chain density in the IPN are helpful for toughening hydrogels, while the semi‐IPN network is beneficial to improve the energy dissipation efficiency.     

Mechanical and tribological behaviors of PVA/PAAm double network hydrogels under varied strains as cartilage replacement

The strain change of double network (DN) hydrogels during compressive mechanical and frictional tests is crucial for their performances. The positive effect of the sacrificed network for prohibiting crack in DN hydrogel is likely to be initiated by large strain. In this study, the mechanical and tribological properties of polyvinyl alcohol/polyacrylamide (PVA/PAAm) DN hydrogels are investigated from the viewpoint of strain. The compressive tangent modulus of PVA/PAAm DN hydrogel with 15 wt% AAm shows a sudden increase in the strain of 60% due to the sacrificed PAAm network. The optimized friction behavior is obtained from PVA/PAAm hydrogel with 5 wt% of AAm content, which is not consistent with the optimal compressive modulus at 15 wt% of AAm content. The variation of frictional coefficient of PVA/PAAm DN hydrogels with load is quite different for migrating and stationary contact configurations. The biphasic lubrication mechanism transited to solid–solid contact dominant mechanism is also induced by the high strain at heavy load.     

Studies on preparation and swelling properties of the N-isopropylacrylamide/chitosan semi-IPN and IPN hydrogels

Semi-interpenetrating network (semi-IPN) polymer gels and interpenetrating network (IPN) polymer gels with thermosensitivity were prepared by introducing a biodegradable polymer, chitosan, into the N-isopropyacrylamide (PNIPAAm) gel system. The swelling behavior, temperature sensitivity, pH sensitivity, gel strength, and drug-release behavior of PNIPAAm/chitosan semi-IPN and IPN hydrogels were investigated. The results indicated that the NIPAAm/chitosan semi-IPN and IPN hydrogels exhibited pH and temperature-sensitivity behavior and could slow drug release and diffusion from the gels. From the stress–strain curves of the hydrogels, the compression moduli of IPN gels containing crosslinked chitosan were higher than those of semi-IPN gels. This is because IPN gels have a more compact structure. The morphology of PNIPAAm/chitosan hydrogels was also investigated. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 82: 2487–2496, 2001     

Electrical/pH responsive properties of poly(2‐acrylamido‐2‐methylpropane sulfonic acid)/hyaluronic acid hydrogels

Poly(2‐acrylamido‐2‐methylpropane sulfonic acid) (PAMPS)/hyaluronic acid (HA) interpenetrating polymer network (IPN) hydrogels have been prepared by using the sequential‐IPN method. The IPN hydrogels exhibited swelling behavior in solutions at various pHs, in NaCl solutions, and under electrical DC stimulation. The IPN hydrogels were highly swollen in water, but lost much of their water capacity when transferred to solutions having a high ionic strength. The IPN hydrogels showed a significant responsive deswelling in an applied electric field. This behavior indicates the potential application of IPN hydrogels as biomaterials. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 92: 1731–1736, 2004     

A novel fabrication method of temperature-responsive poly(acrylamide) composite hydrogel with high mechanical strength

High strength, stimuli-responsive poly(acrylamide) composite hydrogels (PAAm CH gels) were prepared by grafting polymerization of acrylamide (AAm) onto temperature-sensitive core–shell microgels. These microgels, composing of poly(N-isopropylacrylamide) as core and polyvinylamine (PVAm) as shell, were used as both initiator and crosslinker to form a robust three-dimensional network via bonding the poly(acrylamide) (PAAm) backbone. The CH gels exhibited a remarkably rapid shrinking rate and transmittance switch in response to the environmental temperature change, which the conventional chemically cross-linking PAAm hydrogels (PAAm OR) were short of. Even compared to the bulk PNIPAAm hydrogels (PNIPAAm OR) crosslinked with N,N′-methylenebisacrylamide (MBA), the CH gels were featured with faster responsive rate, which could be attributed to the formation of interconnected water transportation channels between the microspheres and PAAm gel matrix due to the fast shrinking of microgels. Moreover, the effects of microgel species and content on swelling and mechanical properties of CH gels were also systematically investigated. The results elaborated that the CH gels could be compressed almost 99% without breaking and completely recovered their original shape when the stress was removed. And the optimized compressive strength of CH gels could be up to 21.94 MPa. Based on the analysis of CH gel mechanical properties, the influence of microsphere content on effective network chains density of CH gels was discussed through rheology measurements. Finally, the essential reinforcement on mechanical properties was mainly contributed to the homogeneous microstructure of hydrogel network and the energy dissipation mechanism of microgels in gel matrix.     

Effects of gamma sterilization on the physicomechanical and thermal properties of gelatin‐based novel hydrogels

Hydrogels are attracting ample attention for tissue engineering application thanks to their water‐loving attribute and closely mimicry to the natural extracellular matrix. However, effectively and efficiently sterilization of hydrogels without compromising their end‐use beneficial attributes is a major challenge. The aim of this work is to study the resistance to gamma sterilization of newly developed gelatin‐based hybrid hydrogels for tissue engineering. This study reported the investigation of 25 kGy gamma sterilization, a typical sterilization procedure for healthcare products, on the physicomechanical and thermal properties of a three set of gelatin‐based novel hydrogels, namely, gelatin–polyethylene glycol (G/PEG), G–PEG–hydroxyethyl cellulose (G/PEG/HEC), and G–PEG–chitosan (G/PEG/CH). Fourier transform infrared and thermogravimetric analysis were done to evaluate the chemical change and variation of thermal behavior, respectively, imposed by the gamma exposure, and the results showed that gamma sterilization did not modify the chemical composition and thermal degradation behavior of the hydrogels. The water uptake, mechanical properties (both in tension and compression), and stress relaxation experiments revealed that parent G/PEG and interpenetrating polymer network (IPN) G/PEG/CH were nearly negligibly sensitive to the gamma sterilization. However, semi‐IPN G/PEG/HEC appeared to be slightly vulnerable to the gamma exposure: a decrease in modulus and strength but simultaneous increase in water uptake, percentage dissipation energy, and stress relaxation responses were observed. POLYM. ENG. SCI., 59:2533–2540, 2019. © 2019 Society of Plastics Engineers     

Enhanced adsorption properties of interpenetrating polymer network hydrogels for heavy metal ion removal

In this study, sequential interpenetrating polymer network (IPN) hydrogels based on poly(polyethylene glycol diacrylate) poly(PEGDA) and poly(methacrylic acid) (PMAA) were prepared with enhanced adsorption properties for heavy metal ion removal. The swelling behavior and mechanical property of the IPN hydrogels were characterized. It was found that swelling ratio increased, and mechanical strength decreased with the PMAA content in the IPN. The IPN hydrogels were used to remove heavy metal ions from aqueous solution under the non-competitive condition. The effects of pH values of the feed solution at the range of 3–5 and PMAA content in the IPN on the adsorption capacity were investigated. The results indicated that the adsorption capacity of the IPN hydrogels increased with the pH values and PMAA content in the IPN. Furthermore, the synergistic complexation of metal ions with two polymer networks in the IPN was found in the adsorption studies. Regeneration studies suggested that metal rebinding capacity of the IPN hydrogels did not change significantly through repeated applications compared with the first run. It was concluded that the poly(PEGDA)/PMAA hydrogels could be used as fast-responsive, high capacity, and renewable sorbent materials in heavy metal removing processes.     

Super-tough hydrogels using ionically crosslinked networks

Alginate and polyacrylamide hydrogels were produced by a facile one-pot method with varied ionic crosslinkers in this article. These hydrogels display outstanding mechanical properties compared to the pristine polyacrylamide (PAAm) hydrogels. The alginate network is ionically crosslinked by multivalent cation, whereas N,N′-methylenebis (acrylamide) (MBAA) is used as covalent crosslinker for the PAAm network. Particularly, the obtained hydrogels by using trivalent cations (Fe³⁺ and Al³⁺) as crosslinkers are much stronger than that of using divalent cations (Ca²⁺ and Ba²⁺) as crosslinkers. In addition, with increasing concentration of cations, the compressive properties of gels are improved, whereas when the concentration is higher than 0.3 M, the compressive properties of gels are damaged due to mono-bindings. Interestingly, the hydrogels with higher chemical crosslinker concentration depicts better mechanical properties than those hydrogels with lower chemical crosslinker, which is different from that of common double network hydrogels. These hydrogels with excellent mechanical properties are promising candidates for biomedical application like load-bearing tissues. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 48182.     

Fabrication of alginate/sericin/cellulose nanocrystals interpenetrating network composite hydrogels with enhanced physicochemical properties and biological activity

Sodium alginate (SA) possesses good biocompatibility and can form hydrogel materials under certain conditions, which has been widely used in tissue engineering. However, the absence of cellular recognition sites and low mechanical strength for single-component alginate (ALG) hydrogels limit their practical applications. Therefore, enhancing the shortcomings of ALG hydrogels and augmenting their characteristics hold immense importance for their medical uses. In this study, comprehensively considering the excellent properties of cellulose nanocrystals (CNCs) and sericin (SS), the alginate/sericin/cellulose nanocrystalline (ALG/SS/CNCS) composite hydrogels were constructed by interpenetrating network (IPN) technique using hydroxyapatite/D-glucono-δ-lactone (HAP/GDL) as the endogenous ionic cross-linking agent of SA, 1-ethyl-(3-dimethylaminopropyl) carbodiimide hydrochloride/N-hydroxysuccinimide (EDC/NHS) as the chemical covalent cross-linking agent of SS and CNCS as the reinforcing agent. The effects of SS and CNCs additions on the comprehensive properties of ALG/SS/CNCs composite hydrogels, such as their morphologies, structure, mechanical properties, swelling, degradability, and cytocompatibility were investigated. The findings indicated that the ALG/SS/CNCS IPN composite hydrogels which were created through the physical blending of SA and SS, displayed a consistent three-dimensional form and a porous configuration. The weak mechanical strength of pure ALG hydrogels can be effectively improved and the swelling stability and mechanical properties of the composite hydrogels can be enhanced through the construction of IPN network and the incorporation of CNCs, thanks to the presence of intermolecular hydrogen bonding. The biodegradability of ALG/SS/CNCS composite hydrogels increased as the SS content increased, indicating that SS facilitated their biomineralization due to its inherent susceptibility to degradation. The results of the cell compatibility test conducted in a laboratory setting showed that SS and CNCS had the ability to enhance the attachment, proliferation, and differentiation of MC3T3-E1 cells on the ALG/SS/CNCS composite hydrogels. Hence, incorporating SS and CNCS into the alginate matrix to create IPN composite hydrogels could significantly enhance the physicochemical and biological characteristics of ALG hydrogels, thus rendering them appropriate for tissue engineering purposes.     

The usability of (sodium alginate/acrylamide) semi-interpenetrating polymer networks on removal of some textile dyes

In this study, (sodium alginate/acrylamide) interpenetrating polymer networks ((NaAlg/AAm)IPN) have been prepared at definite composition. The aqueous solution of 3% (w/v) sodium alginate and 50% (w/v) acrylamide was irradiated with ⁶⁰Co-γ rays at a dose rate of 0.07 kGy/h up to 5 kGy. The percent conversion was determined gravimetrically and 100% gelation was achieved at 5 kGy dose. To understand whether the semi-interpenetrating polymer network of sodium alginate is performed, Fourier Transform Infrared (FTIR) spectra of polyacrylamide (PAAm), sodium alginate, and the semi-interpenetrating polymer network were recorded. It is found that the FTIR spectra of PAAm, NaAlg, and the semi-interpenetrating polymer network are different. The thermograms of PAAm, sodium alginate, and the semi-interpenetrating polymer network were recorded for investigating their thermal character. (NaAlg/AAm)IPN hydrogels were immersed to swell in a solution of pH 7, at a temperature of 25°C. The swelling results at pH 7.0 indicated that (NaAlg/AAm)IPN hydrogel, containing 3% NaAlg showed maximum % swelling in water but swelling increased in the order of water > Magenta > Methylene Blue > Safranine-O > Methyl Violet. Diffusion of water and aqueous solution of dyes within (NaAlg/AAm)IPN hydrogels was found to be of Fickian character at the initial stage of swelling with regard to values calculated for diffusion coefficient of (NaAlg/AAm)IPN hydrogels in water and aqueous solution of dyes. Some diffusion parameters were calculated from swelling of (NaAlg/AAm)IPN in water and dyes and their adsorption isotherms were plotted. In the adsorption experiments, the efficiency of (NaAlg/AAm)IPN hydrogels to adsorb Magenta, Safranine-O, Methylene Blue, and Methyl Violet dyes from water was studied. (NaAlg/AAm)IPN hydrogels showed different adsorption for different aqueous solution of dyes at pH 7.0. Adsorption isotherms were constructed for (NaAlg/AAm)IPN-dye systems. S type adsorption in the Giles classification system was found. Thermal and spectroscopic characterization of semi-interpenetrating polymer network of sodium alginate and acrylamide and dye adsorbed semi-interpenetrating polymer network of sodium alginate and acrylamide was recorded. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Synthesis,characterization, and cytotoxicity of PCL–PEG–PCL diacrylate and agarose interpenetrating network hydrogels for cartilage tissue engineering

Hydrogels are suitable biomaterials for cartilage tissue engineering due to the excellent ability to retain water to provide suitable environment for the tissue, however, the insufficient mechanical properties often prevent their wider applications. The objective of this study was to fabricate biocompatible hydrogels with good mechanical performance, high-water content, and porous microstructure for cartilage regeneration. Photocrosslinked hydrogels are one of the most widely used systems in tissue engineering due to the superior mechanical properties. In this study, block copolymer, poly(ε -caprolactone)-poly(ethylene)-poly(ε -caprolactone) diacrylate (PCL–PEG–PCL; PEC), was prepared by ring-opening polymerization, and PEC hydrogels were made through free radical crosslinking mechanism. Agarose network is chosen as another component of the hydrogels, because of the high-swelling behavior and cartilage-like microstructure, which is helpful for chondrocytes growth. Interpenetrating networks (IPN) were fabricated by diffusing PEC into agarose network followed by photo-crosslinking process. It was noted that incorporating PEC into the agarose network increased the elastic modulus and the compressive failure properties of individual component networks. In addition, high-swelling ratio and uniform porosity microstructures were found in the IPN hydrogels. IPN and PEC showed low cytotoxicity and good biocompatibility in elution test method. The results suggest promising characteristics of IPN hydrogels as a potential biomaterial for cartilage tissue engineering.     

Preparation and characterization of tough and highly resilient nanocomposite hydrogels reinforced by surface-grafted cellulose nanocrystals

Despite many strong and tough hydrogels have been fabricated according to the energy dissipating mechanism, they usually lack high resilience due to the presence of large hysteresis. Herein, poly (N-vinylpyrrolidone) grafted cellulose nanocrystal (CNC-g-PVP) was used as special multifunctional physical crosslinkers to fabricate tough and highly resilient nanocomposite hydrogels. CNC-g-PVP with varying loading was incorporated into chemically crosslinked polyacrylamide (PAM) networks by in-situ radical polymerization to give PAM/CNC-g-PVP nanocomposite hydrogels. Robust cooperative hydrogen bonds existed between the surface-grafted PVP chains and the PAM matrix, which could rupture to dissipate energy upon deformation and recover instantly on the removal of stress. This unique energy dissipating mechanism led to excellent mechanical performance of the hydrogels. Their tensile elastic modulus, toughness, and compressive strength are 1.4–1.8, 2.1–3.0, and 1.44–2.73 times of pure PAM hydrogel, respectively. Moreover, the hydrogels exhibit low hysteresis, high resilience (ca. 97%) under cyclic tensile loading-unloading and good recovery of hysteresis (ca. 90%) under cyclic compressive loading-unloading.     

Super Bulk and Interfacial Toughness of Amylopectin Reinforced PAAm/PVA Double‐Network Hydrogels via Multiple Hydrogen Bonds

A simple, multiple‐hydrogen‐bond approach to fabricating physically crosslinked, Amylopectin reinforced polyacrylamide/poly(vinyl alcohol) (Amy/PAAm/PVA) double‐network (DN) hydrogels with super toughness in bulk and at solid interfaces is reported. The Amy/PAAm/PVA DN hydrogels exhibit high tensile strength (854.1 kPa), high extensibility (≈eight times), high bulk toughness (4094.8 kJ m^?3), good self‐recovery property (≈92% of self‐recovery at room temperature), and strong adhesion to nonporous glass surfaces (≈158 kPa). Such tough and adhesive DN hydrogels have great potential for various applications in engineering artificial soft tissues, flexible electronics, and wearable devices.     

Water-swellable,tough, and stretchable inorganic–organic sulfoaluminate cement/polyacrylamide double-network hydrogel composites

Effectively improving the mechanical properties of the hydrogel can greatly broaden its application range. The design concept of forming a double-network structure by organic–inorganic hybridization can greatly enhance the mechanical properties of traditional hydrogels. Here, a series of organic–inorganic double-network (OIDN) polyacrylamide/(sulfoaluminate cement) (PAM/SAC) composite gels by solution polymerization were synthesized at room temperature. The OIDN composite gels not only retain the characteristics of water swelling but also exhibit excellent tensile properties (stress and strain are 12 MPa and 2500%, respectively) and compressive strength (stress and strain are 65 MPa and 80%, respectively). In the preparation process, a brittle inorganic network of hydrated sulfoaluminate (hydra-SAC) and a ductile network of polyacrylamide (PAM) were formed by the manner of interpenetrating. The phase composition and thermal stability of the OIDN composite gels were characterized and determined by FTIR, XRD, SEM, and TGA, respectively. The effect of SAC on swelling and mechanical performance of the OIDN composite gels was also investigated. The results show that the use of SAC hybrid hydrogels can effectively improve the mechanical strength, and the OIDN composite gels are expected to be a potential grouting and plugging functional material. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 47905.     

Preparation and characterization of PAM/SA tough hydrogels reinforced by IPN technique based on covalent/ionic crosslinking

In order to fabricate tough hydrogels with superior formability, polyacrylamide/sodium alginate (PAM/SA) interpenetrating polymer network (IPN) hydrogels were produced with ionically crosslinked SA interpenetrated in covalently crosslinked PAM. TGA results show that the heat resistance of PAM/SA IPN hydrogel is improved as compared to that of the individual component. Swelling studies indicate that increasing either chemical crosslinker content or ionic crosslinking via adding more N,N′‐methylenebisacrylamide (MBA) or SA results in lower ESR. It is concluded by tensile test that loosely crosslinked PAM coupled with tightly crosslinked SA improve mechanical strength for hydrogels based on covalent/ionic crosslinking. PAM/SA hydrogels via “one‐pot” method can form different complex shapes with mechanical properties comparable to conventional double network (DN) gels. The fracture strength of PAM_0.05/SA₂₀ reaches level of MPa, approaching 2.0 MPa. The work strives to provide method to tune mechanical and physical properties for hydrogels, which is hopefully to guide the design of hydrogel material with desirable properties. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41342.     

Effect of the sodium dodecyl sulfate/monomer ratio on the network structure of hydrophobic association hydrogels with adjustable mechanical properties

The study of gel‐network structure is not as extensive as the study of the application of hydrogels. However, the distribution of the inner structure is crucial for designing hydrogels with tunable mechanical properties to meet certain kinds of demands. In this study, a series of hydrophobic association hydrogels (HA‐gels) were synthesized by free‐radical micellar copolymerization in a sodium dodecyl sulfate (SDS) surfactant solution. The hydrophobic monomer was palmityl alcohol poly(oxyethylene acrylate) (AEO–AC), which is an ecofriendly alternative to the traditional octyl phenol poly(oxyethylene acrylate). Interestingly, we found that the molar ratio [or ratio point (R)] of SDS to AEO–AC played a key role in tuning the mechanical properties. All series HA‐gels denominated a similar down–up–down tendency with increasing R, and the best R is 3. This result was consistent with the microscopic network structure number of the hydrophobic monomer (N_H = 21–24), and this indicated that each hydrophobic monomer associated three SDS monomers in its internal networks. The resulting AEO–AC–acrylamide gels exhibited the best mechanical strength (yield maximum broken stress = 218 kPa) and the maximum effective crosslink density. Moreover, the relationship between the network structure and the mechanical properties of the HA‐gels was investigated with various Rs. Two different interaction effects of distribution between SDS and AEO–AC are discussed in detail. The HA‐gels exhibited self‐healing properties and maintained their shape in water over 160 days. The results indicate that changing R is an effective method for tuning the mechanical properties of HA‐gels as a type of prospective biomedical material. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2017 , 134, 45196.     

Preparation of alginate/poly(N‐isopropylacrylamide) semi‐interpenetrating and fully interpenetrating polymer network hydrogels with γ‐ray irradiation and their swelling behaviors

Semi‐interpenetrating polymer network (semi‐IPN) and fully interpenetrating polymer network (full‐IPN) hydrogels composed of alginate and poly(N‐isopropylacrylamide) were prepared with γ‐ray irradiation. The semi‐IPN hydrogels were prepared through the irradiation of a mixed solution composed of alginate and N‐isopropylacrylamide (NIPAAm) monomer to simultaneously achieve the polymerization and self‐crosslinking of NIPAAm. The full‐IPN hydrogels were formed through the immersion of the semi‐IPN film in a calcium‐ion solution. The results for the swelling and deswelling behaviors showed that the swelling ratio of semi‐IPN hydrogels was higher than that of full‐IPN hydrogels. A semi‐IPN hydrogel containing more alginate exhibited relatively rapid swelling and deswelling rates, whereas a full‐IPN hydrogel showed an adverse tendency. All the hydrogels with NIPAAm exhibited a change in the swelling ratio around 30–40°C, and full‐IPN hydrogels showed more sensitive and reversible behavior than semi‐IPN hydrogels under a stepwise stimulus. In addition, the swelling ratio of the hydrogels continuously increased with the pH values, and the swelling processes were proven to be repeatable with pH changes. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 100: 4439–4446, 2006     

The swelling behaviors and network parameters of cationic starch‐g‐acrylic acid/poly(dimethyldiallylammonium chloride) semi‐interpenetrating polymer networks hydrogels

Amphiphilic semi‐interpenetrating polymer networks (semi‐IPN) hydrogels were prepared by a sequential‐IPN method by acrylic acid graft copolymerization into cationic starch in mild aqueous media of poly(dimethyldiallylammonium chloride). Some main factors were investigated to evaluate the swelling of hydrogels, and the network parameters M_c were given accordingly to elaborate the interaction between polymers. The chemical structure of the resulting hydrogel was confirmed using Fourier transform infrared spectroscopy. The cationic starch‐based semi‐IPN hydrogels achieved a high swelling capacity of 1070 g/g in deionized water and 94 g/g in 0.9 wt % NaCl solution, respectively) and high compressive stress in a high water content. Besides, a different pH‐dependent behavior was found for this semi‐IPN hydrogel. © 2008 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Mechanical properties of interpenetrating polymer network hydrogels based on hybrid ionically and covalently crosslinked networks

Hydrogels are polymer networks swollen in water. Because of their soft and wet nature, and their ability to show large volume changes, hydrogels can be useful in many biomedical and actuator applications. In these applications, it is crucial to tune the mechanical and physical properties of a hydrogel in a controllable manner. Here, interpenetrating polymer networks (IPNs) made of a covalently crosslinked network and an ionically crosslinked network were produced to investigate the effective parameters that control the physical and mechanical properties of an IPN hydrogel. Covalently crosslinked polyacrylamide (PAAm) or poly(acrylic acid) (PAA) networks were produced in the presence of alginate (Alg) that was then ionically crosslinked to produce the IPN hydrogels. The effect of ionic crosslinking, degree of covalent crosslinking, AAm : Alg and AA : Alg ratio on the swelling ratio, tensile properties, indentation modulus, and fracture energy of IPN hydrogels was studied. A hollow cylindrical hydrogel with gradient mechanical properties along its length was developed based on the obtained results. The middle section of this hydrogel was designed as a pH triggered artificial muscle, while each end was formulated to be harder, tougher, and insensitive to pH so as to function as a tendon‐like material securing the gel muscle to its mechanical supports. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 2504–2513, 2013