Crystallization,mechanical, and fracture behavior of mullite fiber‐reinforced polypropylene nanocomposites

This study describes the reinforcement effect of surface modified mullite fibers on the crystallization, thermal stability, and mechanical properties of polypropylene (PP). The nanocomposites were developed using polypropylene‐grafted‐maleic anhydride (PP‐g‐MA) as compatibilizer with different weight ratios (0.5, 1.0, 1.5, 2.5, 5.0, and 10.0 wt %) of amine functionalized mullite fibers (AMUF) via solution blending method. Chemical grafting of AMUF with PP‐g‐MA resulted in enhanced filler dispersion in the polymer as well as effective filler‐polymer interactions. The dispersion of nanofiller in the polymer matrix was identified using scanning electron microscopy (SEM) elemental mapping and transmission electron microscopy (TEM) analysis. AMUF increased the Young's modulus of PP in the nanocomposites up to a 5 wt % filler content, however, at 10 wt % loading, a decrease in the modulus resulted due to agglomeration of AMUF. The impact strength of PP increased simultaneously with the modulus as a function of AMUF content (up to 5 wt %). The mechanical properties of PP‐AMUF nanocomposites exhibited improved thermal performance as compared to pure PP matrix, thus, confirming the overall potential of the generated composites for a variety of structural applications. The mechanical properties of 5 wt % of AMUF filled PP nanocomposite were also compared with PP nanocomposites generated with unmodified MUF and the results confirmed superior mechanical properties on incorporation of modified filler. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43725.     

Graphene nanoplatelet‐reinforced semi‐crystal poly(arylene ether nitrile) nanocomposites prepared by the twin‐screw extrusion

Graphene nanoplatelet reinforced semi‐crystal poly(arylene ether nitrile) (PEN/GN) nanocomposites were prepared by an economically and environmentally friendly method of twin‐screw extrusion technique. The feasibility of using PEN/GN nanocomposites was investigated by evaluating their thermal behaviors, mechanical, and morphological properties. Thermal studies revealed that GN could act as nucleating agents but decreased the whole crystallinity in/of PEN/GN nanocomposites. Mechanical investigation manifested that GN had both strengthening effect (increase in flexural modulus and strength) and toughening effect (rise in the elongation and impact strength) on the mechanical performance of semi‐crystal PEN nanocomposites. Heat treatment can further increase their mechanical performances due to the increased crystallinity and release of inner stress. With the small addition of GN (<5 wt%), the morphology of PEN was changed from brittle to ductile, and GN showed good dispersion and adhesion in/to the PEN matrix. This work shows that in the semi‐crystal polymer/filler systems, besides the dispersion states of fillers and interactions between fillers and polymer matrices, the crystallinity of the nanocomposites affected by the existence of filler and the residual stress are also two key factors determining the mechanical properties. POLYM. COMPOS., 35:404–411, 2014. © 2013 Society of Plastics Engineers     

Investigation of thermomechanical properties and matrix–filler interaction on polyimide/graphene oxide composites

We report, the preparation of nanocomposites having polyimide (PI) as matrix and graphene oxide (GO) as filler, analyses of matrix–filler interactions, and enhancements in thermomechanical properties of PI/GO as compared with pristine PI. The matrix–filler interactions were analyzed by ¹H NMR, X‐ray photoelectron spectroscopy, and density functional theory calculations. The data suggested stronger matrix–filler interactions in PI/GO as compared with PI/G composites. The stronger matrix–filler interactions and homogeneous dispersion of fillers lead to a significant enhancement in mechanical properties in PI/GO nanocomposites. Thus, with just 1 wt% GO content, the modulus of PI/GO composite increased by ～106% as compared with pristine PI. Finally, thermal expansion coefficients of the nanocomposites are also investigated. A plausible hypothesis has been proposed in the text to explain the observed matrix–filler interactions and the subsequent property enhancements in nanocomposites. POLYM. ENG. SCI., 2012. © 2012 Society of Plastics Engineers     

Studies on engineering properties of PVC–PMMA semi‐interpenetrating polymer networks

Semi1 and semi2 interpenetrating polymer networks (IPNs) of PVC and in situ formed PMMA have been synthesized using diallyl phthalate and ethylene glycol dimethacrylate as the crosslinkers of PVC and PMMA, respectively. These two types of IPNs have been compared w.r.t their physical, mechanical, and thermal properties and an endeavor has been made to find a correlation of these properties with the morphology generated in these systems. The semi1 IPNs displayed a decrease in their mechanical parameters and the physical properties as well, while in contrast, the semi2 IPNs exhibited a marginal increase in the corresponding values after an initial drop upto about 15% of crosslinked PMMA incorporation when compared to the crosslinked PVC in the case of semi1 IPN and linear PVC in the case of semi2 IPN. The various samples of semi1 and semi2 IPNs showed a two‐stage degradation typical of PVC, while confirming the increased stability with the samples having higher percentages of PMMA. The influence of crosslinking of the major matrix in semi1 IPN was almost counterbalanced by the influence of crosslinking in the dispersed PMMA phase in the case of semi2 IPN. The softening characteristics as detected by the extent of penetration of the probe, as has been detected by thermomechanical analysis, are in conformity with their mechanicals. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 97: 1725–1735, 2005     

Miscibility and properties of semi‐interpenetrating polymer networks based on polyurethane and nitroguar gum

Films from castor oil‐based polyurethane (PU) prepolymer and nitroguar gum (NGG) with different contents (10–70 wt %) were prepared through solution casting method. The networks of PU crosslinked with 1,4‐butanediol were interpenetrated by linear NGG to form semi‐interpenetrating polymer networks (semi‐IPNs) in the blend films. The miscibility, morphology, and properties of the semi‐IPNs coded as PUNG films were investigated with Fourier transform infrared spectroscopy, scanning electron microscopy, differential scanning calorimetry, dynamic mechanical thermal analysis, wide‐angle X‐ray diffraction, density measurement, ultraviolet spectroscopy, thermogravimetric analysis, tensile, and solvent‐resistance testing. The results revealed that the semi‐IPNs films have good miscibility over the entire composition ratio of PU to NGG under study. The occurrence of hydrogen‐bonding interaction between PU and NGG played a key role in improvement of the material performance. Compared with the pure PU film, the PUNG films exhibited higher values of tensile strength (11.7–28.4 MPa). Meanwhile, incorporating NGG into the PU networks led to an improvement of thermal stability and better solvent‐resistance of the resulting materials. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci 104, 4068–4079, 2007     

Semi‐interpenetrating polymer networks based on polyurethane and poly(vinyl pyrrolidone) obtained by photopolymerization: Structure‐property relationships and bacterial adhesion

A range of semi‐interpenetrating polymer networks (semi‐IPNs) based on polyurethane (PU) and poly(vinyl pyrrolidone) (PVP) have been synthesized and characterized with respect to their thermodynamic characteristics, morphology, mechanical properties, surface properties, water sorption and bacterial adhesion. The free energies of mixing of PU and PVP in semi‐IPNs have been determined by the vapor sorption method and were shown to be positive for all compositions. The surface properties of semi‐IPNs were investigated using the dynamic contact angle analysis. It was shown that the advancing contact angle changes from 83.1° to 65.3° with increasing PVP from 7.05% to 57.38%. Scanning electron microscopy demonstrated that the semi‐IPNs are two‐phase systems with incomplete phase separation. The mechanical properties reflect the changes in structure of semi‐IPNs with increasing of amounts of PVP in the system. Incorporation of PVP into the semi‐IPN with PU restricts the ability of PVP to sorb water. As infection is likely to be caused by bacterial adherence to biomedical implants, the bacterial adhesion data suggests that the semi‐IPNs with PVP content below 22.52% may be useful for biomedical material applications. Polym. Eng. Sci. 44:940–947, 2004. © 2004 Society of Plastics Engineers.     

Insolubilization of sodium chondroitin sulfate by forming a semi‐interpenetrating polymer network with acrylic acid: A potential carrier for colon‐specific drug delivery

To reduce the highly hydrophilic property of chondroitin sulfate (ChS), a semi‐interpenetrating polymer network (semi‐IPN) of chondroitin sulfate/polyacrylic acid (PAA) was prepared as a drug carrier by crosslinking acrylic acid with diethyleneglycol diacrylate. The swelling properties of the semi‐IPNs with different concentrations of crosslinking agent were correlated. The moisture sorption profiles were evaluated using differential thermal analysis. Ketoprofen was used as a drug probe to evaluate the performance of the drug released from the semi‐IPN matrices. The prepared semi‐IPNs demonstrated significant swelling reduction properties with both gastric and intestinal fluids compared with those of both the pure ChS and the ChSAA blend without the crosslinking agent. The amount of accumulated drug released from the semi‐IPNs was less than 30 wt % at pH 1.2 and up to 80 wt % at pH 7.4. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 85: 114–122, 2002     

Properties of poly(vinyl alcohol)—Bentonite clay nanocomposite films in relation to polymer–clay interactions

This study describes an effective way for the preparation of well‐dispersed, high‐loaded PVA/bentonite nanocomposites with improved properties, based on nanoscale interactions. To this end, a series of Poly(vinyl alcohol)—bentonite clay nanocomposites have been prepared via solvent casting technique and their properties were thoroughly investigated by atomic force microscopy, transmission electron microscopy, X‐Ray diffraction, oxygen and water permeability, water sorption along with mechanical and thermal studies. Microscopic and XRD techniques revealed highly organized regions. Clay content up to 10% led to nanocomposites with high degree of exfoliation. In addition samples with increased filler content (20%) demonstrated also, apart from the delaminated, well‐organized intercalated regions. The nanocomposites exhibited increased mechanical, thermal and gas barrier properties, though they retained their optical clarity. Thus, the Young's modulus of the sample containing 20% clay was increased by 193 times, while the oxygen permeability was decreased about seven times, in regard to the corresponding values of the neat polymer. The obtained results were explored on the basis of nanoscale phenomena and it was concluded that the organized structures and intercalated regions observed on highly loaded samples are attributed to the competitive effect between weaker polymer–polymer interactions in relation to stronger polymer–clay ones. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Semi‐interpenetrating polymer networks based on polyurethane and polyvinylpyrrolidone. II. Dielectric relaxation and thermal behaviour

Semi‐interpenetrating polymer networks (semi‐IPNs) based on crosslinked polyurethane (PU) and linear polyvinylpyrrolidone (PVP) were synthezised, and their thermal and dynamic mechanical properties and dielectric relaxation behavior were studied to provide insight into their structure, especially according to their composition. The differential scanning calorimetry results showed the glass transitions of the pure components: one glass‐transition temperature (T_g) for PU and two transitions for PVP. Such glass transitions were also present in the semi‐IPNs, whatever their composition. The viscoelastic properties of the semi‐IPNs reflected their thermal behavior; it was shown that the semi‐IPNs presented three distinct dynamic mechanical relaxations related to these three T_g values. Although the temperature position of the PU maximum tan δ of the α‐relaxation was invariable, on the contrary the situation for the two maxima observed for PVP was more complex. Only the maximum of the highest temperature relaxation was shifted to lower temperatures with decreasing PVP content in the semi‐IPNs. In this study, we investigated the molecular mobility of the IPNs by means of dielectric relaxation spectroscopy; six relaxation processes were observed and indexed according the increase in the temperature range: the secondary β‐relaxations related to PU and PVP chains, an α‐relaxation due to the glass–rubber transition of the PU component, two α‐relaxations associated to the glass–rubber transitions of the PVP material, and an ionic conductivity relaxation due to the space charge polarization of PU. The temperature position of the α‐relaxation of PU was invariable in semi‐IPNs, as observed dynamic mechanical analysis measurements. However, the upper α‐relaxation process of PVP shifted to higher temperatures with increasing PVP content in the semi‐IPNs. We concluded that the investigated semi‐IPNs were two‐phase systems with incomplete phase separation and that the content of PVP in the IPNs governed the structure and corresponding properties of such systems through physical interactions. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 90: 1191–1201, 2003     

Ultrasound–assisted synthesis and characterization of polymethyl methacrylate/reduced graphene oxide nanocomposites

This article reports ultrasound–assisted synthesis of polymethyl methacrylate (PMMA)/reduced graphene oxide (RGO) nanocomposites by in situ emulsion polymerization coupled with in situ reduction of graphene oxide. The thermal degradation kinetics of the nanocomposites was also assessed with Criado and Coats‐Redfern methods. Intense microconvection generated by ultrasound and cavitation results in uniform dispersion of RGO in the polymer matrix, which imparts markedly higher physical properties to resulting nanocomposites at low (≤1.0 wt %) RGO loadings, as compared to nanocomposites synthesized with mechanical stirring. Some important properties of the PMMA/RGO nanocomposites synthesized with sonication (with various RGO loadings) are: glass transition temperature (0.4 wt %) = 124.5°C, tensile strength (0.4 wt %) = 40.4 MPa, electrical conductivity (1.0 wt %) = 2 × 10^?7 S/cm, electromagnetic interference shielding effectiveness (1.0 wt %) = 3.3 dB. Predominant thermal degradation mechanism of nanocomposites (1.0 wt % RGO) is 1D diffusion with activation energy of 111.3 kJ/mol. © 2017 American Institute of Chemical Engineers AIChE J, 64: 673–687, 2018     

Polyethylene–Silica Nanocomposites with the Structure of Semi‐Interpenetrating Networks

Organic–inorganic nanocomposites with the structure of interpenetrating or semi‐interpenetrating networks are considered as advanced materials, since they have improved thermal and mechanical properties. An alternative approach to the preparation of such hybrid systems is proposed. It is based on the synthesis of silica from the precursor of hyperbranched polyethoxysiloxane by the hydrolytic condensation reaction in the volume of pores of a polymer matrix (bulk porosity is 40 vol%) stretched via the environmental crazing mechanism. Polyethylene–silica nanocomposites with the structure of semi‐interpenetrating networks when the content of silica is not less than 20–25 wt% are obtained. These composites can undergo an additional phase separation at a temperature of 160 °C (above the melting point of polyethylene), which is accompanied by an increase in the size of the polymer phase with the formation of macrophases. At the same time, the environment (orthophosphoric acid), in which the composite is heated, fills the pores that have appeared. As a result, the content of the third component with the new functionality increases up to 50 wt%, which allowed us to impart proton‐conducting properties to the composite material and preserve its shape stability.     

Engineering properties of poly(vinyl chloride)–poly(butyl methacrylate) semi‐1 and semi‐2 interpenetrating polymer networks

Semi‐1 and semi‐2 interpenetrating polymer networks (IPNs) of poly(vinyl chloride) (PVC) and in situ formed poly(butyl methacrylate) (PBMA) have been synthesized using diallyl phthalate and ethylene glycol dimethacrylate as the crosslinkers of PVC and PBMA, respectively. These were then characterized with reference to their mechanical, thermal, and morphological properties. The mechanical and thermal characteristics revealed modification over the unmodified polymeric systems in relation to their phase morphologies. The semi‐1 IPNs displayed a decrease in their mechanical parameters of modulus and UTS while semi‐2 IPNs exhibited a marginal increase in these two values. The semi‐1 IPNs, however, also revealed a decrease in the elongation and toughness values away from the normal behavior. The thermomechanical behavior of both the systems is in conformity with their mechanicals in displaying the softening characteristics of the system and stabilization over unmodified PVC. The DSC thermograms are also correlated to these observations along with the heterogeneous phase morphology which is displayed by both the systems especially at higher concentration of PBMA incorporation. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Synergistic effect of three‐dimensional multi‐walled carbon nanotube–graphene nanofiller in enhancing the mechanical and thermal properties of high‐performance silicone rubber

The homogeneous dispersion of nanofillers and filler–matrix interfacial interactions are important factors in the development of high‐performance polymer materials for various applications. In the present work, a simple solution‐mixing method was used to prepare multi‐walled carbon nanotube (MWCNT)–graphene (G) (3:1, 1:1, 1:3) hybrids followed by their characterization through wide‐angle X‐ray diffraction, transmission electron microscopy and thermogravimetric analyses. Subsequently, MWCNT–G (1:1) hybrid was used as reinforcing filler in the formation of silicone rubber (VMQ) nanocomposites by solution intercalation, and their morphology and properties were investigated. Our findings showed that MWCNT–G (0.75 wt%)/VMQ composite exhibited significant improvements in tensile strength (110%) and Young's modulus (137%) compared to neat VMQ. The thermal stability of MWCNT–G (1 wt%)/VMQ was maximally improved by 154 °C compared to neat VMQ. Differential scanning calorimetry demonstrated the maximum improvement of glass transition temperature (4 °C), crystallization temperature (8 °C) and melting temperature (5 °C) for MWCNT–G (1 wt%)/VMQ nanocomposite with respect to neat VMQ. Swelling measurements confirmed that the crosslink density and solvent resistance were a maximum for hybrid nanocomposites. Such improvements in the properties of MWCNT–G/VMQ nanocomposites could be attributed to a synergistic effect of the hybrid filler. © 2013 Society of Chemical Industry     

Phase separation in the polyurethane/poly(2‐hydroxyethyl methacrylate) semi‐interpenetrating polymer networks synthesized by different ways

The thermal, dynamic mechanical analysis, morphology and mechanical properties of semi‐interpenetrating polymer networks based on crosslinked polyurethane (PU) and poly(2‐hydroxyethyl methacrylate) (PHEMA) synthesized by photopolymerization and by thermopolymerization have been investigated. The thermal analysis has evidenced the two glass temperature transitions in the semi‐IPNs and this is confirmed by the thermodynamic miscibility investigation of the systems. The Dynamic Mechanical Analysis spectra have shown that the phase separation is more significant in the thermopolymerized semi‐IPNs: the tan δ peaks of constituent polymers are more distinct and the minimum between the two peaks is deeper. The calculated segregation degree values of semi‐IPN's components are significantly higher for thermopolymerized semi‐IPNs, thereby the process of phase separation in the thermopolymerized semi‐IPNs is more developed. The structures of two series of samples investigated by SEM are completely different. The mechanical properties reflect these changes in structure of semi‐IPNs with increasing amount of PHEMA and with the changing of the method of synthesis. The results suggest that the studied semi‐IPNs are two‐phase systems with incomplete phase separation. The semi‐IPN samples with early stage of phase separation demonstrate higher mechanical characteristics. POLYM. ENG. SCI., 2008. © 2008 Society of Plastics Engineers     

Novolac resin–poly(ethyl methacrylate) interpenetrating polymer networks: Morphology and mechanical and thermal properties

Full interpenetrating networks (IPNs) and semi‐IPNs of Novolac (phenolic) resin and poly(ethyl methacrylate) (PEMA) were prepared by the sequential mode of synthesis. These were characterized with respect to their mechanical properties, that is, ultimate tensile strength (UTS), percentage elongation at break, modulus, and toughness. Thermal properties were studied by DSC and thermogravimetric analysis (TGA). The morphological features were studied through polarizing light microscopy (PLM). The effects of variation of the blend ratios on the above‐mentioned properties were examined. There was a gradual decrease of modulus and UTS with consequent increases in elongation at break and toughness for both types of IPNs with increasing proportions of PEMA. An inward shift and lowering (with respect to pure phenolic resin) of the glass‐transition temperatures of the IPNs with increasing proportions of PEMA were observed, thus indicating a plasticizing influence of PEMA on the rigid and brittle matrix of crosslinked phenolic resin. The TGA thermograms exhibit two‐step degradation patterns. Although there was an apparent increase in thermal stability at the initial stages, particularly at lower temperatures, a substantial decrease in thermal stability was observed in the regions of higher temperatures. The surface morphology as revealed by PLM clearly indicates two‐phase structures in all the full and semi‐IPNs, irrespective of PEMA content. The matrix–PEMA domain interfaces are quite sharp at higher concentrations of PEMA. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 90: 412–420, 2003     

Curing and mechanical properties of dicyanate/poly(ether sulfone) semi‐interpenetrating polymer networks

Semi‐interpenetrating polymer networks (semi‐IPNs) composed of a dicyanate resin and a poly(ether sulfone) (PES) were prepared, and their curing behavior and mechanical properties were investigated. The curing behavior of the dicyanate/PES semi‐IPN systems catalyzed by an organic metal salt was analyzed. Differential scanning calorimetry was used to study the curing behavior of the semi‐IPN systems. The curing rate of the semi‐IPN systems decreased as the PES content increased. An autocatalytic reaction mechanism was used to analyze the curing reaction of the semi‐IPN systems. The glass‐transition temperature of the semi‐IPNs decreased with increasing PES content. The thermal decomposition behavior of the semi‐IPNs was investigated. The morphology of the semi‐IPNs was investigated with scanning electron microscopy. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 87: 1079–1084, 2003     

Bio‐based polymer nanocomposites based on layered silicates having a reactive and renewable intercalant

Soybean oil‐based polymer nanocomposites were synthesized from acrylated epoxidized soybean oil (AESO) combined with styrene monomer and montmorillonite (MMT) clay by using in situ free radical polymerization reaction. Special attention was paid to the modification of MMT clay, which was carried out by methacryl‐functionalized and quaternized derivative of methyl oleate intercalant. It was synthesized from olive oil triglyceride, as a renewable intercalant. The resultant nanocomposites were characterized by X‐ray diffraction (XRD) and transmission electron microscopy (TEM). The effect of increased nanofiller loading in thermal and mechanical properties of the nanocomposites was investigated by thermogravimetric analysis (TGA) and dynamic mechanical analysis (DMA). The nanocomposites exhibited improved thermal and dynamic mechanical properties compared with neat acrylated epoxidized soybean oil based polymer matrix. The desired exfoliated nanocomposite structure was achieved when the OrgMMT loading was 1 and 2 wt % whereas partially exfoliated nanocomposite was obtained in 3 wt % loading. It was found that about 400 and 500% increments in storage modulus at glass transition and rubbery regions, respectively were achieved at 2 wt % clay loading compared to neat polymer matrix while the lowest thermal degradation rate was gained by introducing 3 wt % clay loading. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 2031–2041, 2013     

Interpenetrating polymer networks of bismaleimide and polyether polyurethane–crosslinked epoxy

In this work, we prepared the interpenetrating polymer networks of bismaleimide and polyether-type polyurethane(polyoxypropylene)–crosslinked epoxy (BMI/PU(PPG)–EP IPNs) by employing the simultaneous bulk polymerization technique. The polyurethane (PU)–crosslinked epoxy was identified via infrared (IR) spectra analysis. Also investigated herein were the mechanical properties, including tensile strength, Izod impact strength, and fracture energy (G_IC) of the IPNs with various BMI contents in PU–crosslinked epoxy matrix. In addition, differential scanning calorimetry (DSC) analysis and the thermogravimetric analysis (TGA) were performed to examine the thermal properties of the BMI/PU(PPG)–EP IPNs. In addition, morphology and dynamic mechanical analysis (DMA) of the BMI/PU(PPG)–EP IPNs were also studied. © 1998 John Wiley & Sons, Inc. J Appl Polym Sci 70: 2635–2645, 1998     

New interpenetrating polymer networks based on uralkyd–poly(butyl methacrylate)

A study on two‐component semi‐ and full‐interpenetrating polymer networks (IPNs) of soyabean‐oil based uralkyd resin (UA) and poly(butyl methacrylate) (PBMA) synthesized by a sequential technique, has been conducted. The IPNs obtained are characterized with respect to their mechanical properties, such as tensile strength, percentage elongation and hardness (Shore A). Phase morphology has been studied by scanning electron microscopy. Glass transition studies have been carried out using differential scanning calorimetry. The thermal characterization of the IPNs was undertaken with the aid of thermogravimetric analysis. The apparent densities of these samples have been determined and are compared. The effect of the compositional variation on the above‐mentioned properties was examined. The tensile strength exhibits a sudden rise (approximately three‐fold) for the semi‐ and full‐IPNs with composition UA: PBMA 40% : 60% compared with the UA:PBMA composition of 20% : 40%. © 2001 Society of Chemical Industry     

Semiinterpenetrating polymer networks based on polyurethane and polyvinylpyrrolidone. I. Thermodynamic state and dynamic mechanical analysis

Semiinterpenetrating polymer networks (semi‐IPNs) based on polyurethane (PU) and polyvinylpyrrolidone (PVP) have been synthesized, and their thermodynamic characteristics, thermal properties, and dynamical mechanical properties have been studied to have an insight in their structure as a function of their composition. First, the free energies of mixing of the two polymers in semi‐IPNs based on crosslinked PU and PVP have been determined by the vapor sorption method. It was established that these constituent polymers are not miscible in the semi‐IPNs. The differential scanning calorimetry results evidence the T_g of polyurethane and two T_g for PVP. The dynamic mechanical behavior of the semi‐IPNs has been investigated and is in accordance with their thermal behavior. It was shown that the semi‐IPNs present three distinct relaxations. If the temperature position of PU maximum tan δ is invariable, on the contrary, the situation for the two maxima observed for PVP is more complex. Only the maximum of the highest temperature relaxation is shifted to lower temperature with changing of the semi‐IPNs composition. It was concluded that investigated semi‐IPNs are two‐phase systems with incomplete phase separation. The phase composition was calculated using viscoelastic properties. © 2001 John Wiley & Sons, Inc. J Appl Polym Sci 80: 852–862, 2001