Damping analysis of polyurethane/polyacrylate interpenetrating polymer network composites filled with graphite particles

The graphite‐filled polyurethane/poly(methyl methacrylate‐butyl methacrylate) (PU/P(MMA‐BMA)) semi‐interpenetrating polymer networks (IPNs) were synthesized by sequential method. The influences of graphite particle content and size on the 60/40 PU/P(MMA‐BMA) IPNs were studied. The damping properties of IPN composites were evaluated by dynamic mechanical thermal analysis (DMA) and cantilever beam resonance methods. The mechanical performances were investigated using tensile and hardness devices. DMA results revealed that the incorporation of graphite particles improved damping properties of IPNs significantly. The 5% graphite‐filled IPN composite exhibited the widest temperature range and the highest loss factor (tan δ) when the test frequency was 1 Hz. As to the damping properties covering a wide frequency range from 1 to 3,000 Hz, the addition of graphite particles broadened the damping frequency range (Δf, where tan δ is above 0.3) and increased the tan δ value of IPNs. Among them, the composite with 7.5% graphite showed the best damping capacity. And the hardness and the tensile strength of IPN composites were also improved significantly. POLYM. COMPOS., 2013 © 2013 Society of Plastics Engineers     

The application of bulk polymerized acrylic and methacrylic interpenetrating polymer networks to noise and vibration damping

Novel acrylic/methacrylic interpenetrating polymer networks (IPNs) were examined by dynamic mechanical spectroscopy for their damping capabilities. While simple homopolymers exhibit high damping properties only over a 20–30°C range, multicomponent polymer systems with controlled degree of miscibility, such as IPNs, may exhibit high damping properties over temperature ranges as broad as approximately 100°C. Two series of IPNs based on poly(n-butyl acrylate) and poly(n-butyl methacrylate) were synthesized and the dynamic mechanical properties were investigated using a Rheovibron. Graphite was incorporated into the poly(n-butyl acrylate) homopolymer and a few IPNs to measure the change in the damping properties. For important IPN compositions, tan δ values between 0.4 and 0.85 were observed over a 75°C plus temperature range. Graphite increased the damping properties of poly(n-butyl acrylate) and the IPNs, as indicated by the tan δ values.     

DMA analysis of the damping of ethylene–vinyl acetate/acrylonitrile butadiene rubber blends

The mechanical and damping properties of blends of ethylene–vinyl acetate rubber (VA content > 40% wt) (EVM)/acrylonitrile butadiene rubber (NBR), with 1.4 phr BIPB [bis (tert‐butyl peroxy isopropyl) benzene] as curing agent, were investigated by DMA and DSC. The effect of chlorinated polyvinyl chloride (CPVC), silica, carbon black, and phenolic resin (PF) as a substitute curing agent, on the damping and mechanical properties of EVM/NBR blends were studied. The results showed that 10 phr CPVC did not contribute to the damping of EVM700/NBR blends; Silica could dramatically improve the damping of EVM700/NBR blends because of the formation of bound rubber between EVM700/NBR and silica, which appeared as a shoulder tan δ peak between 20 and 70°C proved by DMA and DSC. This shoulder tan δ peak increased as the increase of the content of EVM in EVM/NBR blends. The tensile strength, modulus at 100% and tear strength of the blend with SiO₂ increased while the elongation at break and hardness decreased comparing with the blend with CB. PF, partly replacing BIPB as the curing agent, could significantly improve the damping of EVM700/NBR to have an effective damping temperature range of over 100°C and reasonable mechanical properties. Among EVM600, EVM700, and EVM800/NBR/silica blend system, EVM800/NBR/silica blend had the best damping properties. The EVM700/NBR = 80/10 blend had a better damping property than EVM700/NBR = 70/20. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Study on the damping of EVM based blends

The mechanical and damping properties of blends of ethylene‐vinyl acetate rubber(VA content >40 wt %) (EVM)/nitrile butadiene rubber (NBR) and EVM/ethylene‐propylene‐diene copolymer (EPDM), both with 1.4 phr BIPB (bis (tert‐butyl peroxy isopropyl) benzene) as curing agent, were investigated by DMA. The effect of polyvinyl chloride (PVC), chlorinated polyvinyl chloride (CPVC), and dicumyl peroxide (DCP) on the damping and mechanical properties of both rubber blends were studied. The results showed that in EVM/EPDM/PVC blends, EPDM was immiscible with EVM and could not expand the damping range of EVM at low temperature. PVC was miscible with EVM and dramatically improved the damping property of EVM at high temperature while keeping good mechanical performance. In EVM/NBR/PVC blends, PVC was partially miscible with EVM/NBR blends and remarkably widened the effective damping temperature range from 41.1°C for EVM/NBR to 62.4°C, while CPVC mixed EVM/NBR blends had an expanded effective damping temperature range of 63.5°C with only one damping peak. Curing agents BIPB and DCP had a similar influence on EVM/EPDM blends. DCP, however, dramatically raised the height of tan δ peak of EVM/NBR = 80/20 and expanded its effective damping temperature range to 64.9°C. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Studies on damping properties of P(MMA‐AN)/P(EA‐nBA) LIPNs

Using a two‐stage emulsion polymerization method, a series of poly(methyl methacrylate‐acrylonitrile)/poly(ethyl acrylate‐n‐butyl acrylate) [P(MMA‐AN)/P(EA‐nBA)] latex interpenetrating polymer networks (LIPNs) were synthesized by varying AN content, ratio of network I/network II, crosslinker content, and introducing chain transfer agent. The damping properties of the LIPNs were investigated using a Rheovibron Viscoelastometer. The results indicates that a suitable content of AN can improve the damping properties of the LIPNs. Three kinds of fillers were incorporated into the LPINs, respectively, to measure the change in the damping properties. Mica and TiO₂ both increased the damping properties of the LIPNs over the wide temperature range. For TiO₂‐filled LIPNs, it was observed that the tan δ values exceeded 0.4 over 112.6°C temperature range from −50 to 72.6°C. © 2000 John Wiley & Sons, Inc. J Appl Polym Sci 76: 722–727, 2000     

Semi‐ and full‐interpenetrating polymer networks based on polyurethane produced from canola oil and poly(methyl methacrylate)

Semi‐ and full‐interpenetrating polymer networks (IPNs) were prepared using polyurethane (PUR) produced from a canola oil‐based polyol with primary terminal functional groups and poly(methyl methacrylate) (PMMA). The properties of the material were studied and compared using dynamic mechanical analysis (DMA), differential scanning calorimetry (DSC), and tensile measurements. The morphology of the IPNs was investigated using atomic force microscopy (AFM). Semi‐IPNs demonstrated different thermal mechanical properties, mechanical properties, phase behavior, and morphology from full IPNs. Both types of IPNs studied are two‐phase systems with incomplete phase separation. However, the extent of phase separation is significantly more advanced in the semi‐IPNs compared with the full IPNs. All the semi‐IPNs exhibited higher values of elongation at break for all proportions of acrylate to polyurethane compared with the corresponding full IPNs. These differences are mainly due to the fact that in the case of semi‐IPNs, one of the constituting polymers remains linear, so that it exhibits a loosely packed network and relatively high mobility, whereas in the case of full IPNs, there is a higher degree of crosslinking, which restricts the mobility of the chains. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Preparation and properties of polyurethane‐modified epoxy cured in different simulated gravity environments

Great attention has been paid to the composites with interpenetrating polymer networks (IPNs) because of their special performance. However, the influence of sedimentation and convection from different gravity environments on the formation of IPNs and the properties of IPNs blends has received little attention. To understand their influence, environments with different gravity accelerations of 0g, 1g, and 2g were simulated with a superconducting magnet, and tests, including differential scanning calorimetry (DSC), dynamic mechanical analysis (DMA), coefficient of thermal expansion (CTE), scanning electron microscopy, and three‐point bending, of the IPNs blends cured in different gravity environments were conducted and analyzed. Fourier transform infrared spectroscopy, DSC, and DMA proved the formation of IPNs during the reaction between the polyurethane prepolymer (PUP) and epoxy resin (E51). The curves of DSC also certified the differences in the curing degree between the different parts along the direction of gravity of a sample. With the increase of mass fraction of PUP, the change trends of the storage modulus presented a linear decrease when samples cured in microgravity environment, but presented a parabolic trend when samples were cured in terrestrial environment. The damping properties of samples cured in simulated microgravity environments are better than those cured in terrestrial environment. With the increase in the simulated acceleration of gravity, the diameter of dispersed phase in a sea‐island structure increased, but their number decreased and the bending stress and CTE of the IPN blends all decreased. These results show the formation of IPNs was affected by different gravity values, and the thermal and mechanical properties of the IPN composites were influenced by the changed IPN components. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42063.     

Transparent poly(methyl methacrylate‐co‐butyl acrylate) nanofibers

Nanofibers of n‐Butyl Acrylate/Methyl Methacrylate copolymer [P(BA‐co‐MMA)] were produced by electrospinning in this study. P(BA‐co‐MMA) was synthesized by emulsion polymerization. The structural and thermal properties of copolymers and electrospun P(BA‐co‐MMA) nanofibers were analyzed using Fourier transform infrared spectroscopy–Attenuated total reflectance (FTIR–ATR), Nuclear magnetic spectroscopy (NMR), and Differential scanning calorimetry (DSC). FTIR–ATR spectra and NMR spectrum revealed that BA and MMA had effectively participated in polymerization. The morphology of the resulting nanofibers was investigated by scanning electron microscopy, indicating that the diameters of P(BA‐co‐MMA) nanofibers were strongly dependent on the polymer solution dielectric constant, and concentration of solution and flow rate. Homogeneous electrospun P(BA‐co‐MMA) fibers as small as 390 ± 30 nm were successfully produced. The dielectric properties of polymer solution strongly affected the diameter and morphology of electrospun polymer fibers. The bending instability of the electrospinning jet increased with higher dielectric constant. The charges inside the polymer jet tended to repel each other so as to stretch and reduce the diameter of the polymer fibers by the presence of high dielectric environment of the solvent. The extent to which the choice of solvent affects the nanofiber characteristics were well illustrated in the electrospinning of [P(BA‐co‐MMA)] from solvents and mixed solvents. Nanofiber mats showed relatively high hydrophobicity with intrinsic water contact angle up to 120°. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 4264–4272, 2013     

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     

Properties and morphologies of elastomer blends modified with EPDM‐g‐poly[2‐dimethylamino ethylmethacrylate]

The graft copolymerization of 2‐dimethylamino ethylmethacrylate (DMAEMA) onto ethylene propylene diene mononer rubber (EPDM) was carried out in toluene via solution polymerization technique at 70°C, using dibenzoyl peroxide as initiator. The synthesized EPDM rubber grafted with poly[DMAEMA] (EPDM‐g‐PDMAEMA) was characterized with ¹H‐NMR spectroscopy, gel permeation chromatography (GPC), differential scanning calorimetry (DSC), and thermal gravimetric analysis (TGA). The EPDM‐g‐PDMAEMA was incorporated into EPDM/butadiene acrylonitrile rubber (EPDM/NBR) blend with different blend ratios, where the homogeneity of such blends was examined with scanning electron microscopy and DSC. The scanning electron micrographs illustrate improvement of the morphology of EPDM/NBR rubber blends as a result of incorporation of EPDM‐g‐PDMAEMA onto that blend. The DSC trace exhibits one glass transition temperature (T_g) for EPDM/NBR blend containing EPDM‐g‐PDMAEMA, indicating improvement of homogeneity. The physico‐mechanical properties after and before accelerated thermal aging of the homogeneous, and inhomogeneous EPDM/NBR vulcanizates with different blend ratios were investigated. The physico‐mechanical properties of all blend vulcanizates were improved after and before accelerated thermal aging, in presence of EPDM‐g‐PDMAEMA. Of all blend ratios under investigation EPDM/NBR (75/25) blend possesses the best physico‐mechanical properties together with the best (least) swelling (%) in brake fluid. Swelling behavior of the rubber blend vulcanizates in motor oil and toluene was also investigated. © 2009 Wiley Periodicals, Inc. J Appl Polym Sci, 2009     

Synthesis and evaluation of fluorosilicone‐modified starch for protection of historic stone

Starch is sensitive to moisture and is weak to durability in the protection application to ancient relics. Therefore, two fluorosilicone‐modified starches are firstly prepared and evaluated for the protection of historic stones. The fluoro‐silicone copolymer grafted starch of P(VTMS/12FMA)‐g‐starch is synthesized by grafting copolymer of vinyltrimethoxysilane (VTMS) and dodecafluoroheptyl methacrylate (12FMA) onto starch. While the fluoro‐silicone starch latex of VTMS‐starch@P(MMA/BA/3FMA) is obtained by emulsion polymerization of VTMS primarily grafted‐starch (VTMS‐starch) with methyl methacrylate (MMA), butyl acrylate (BA) and 2,2,2‐trifluoroethyl methacrylate (3FMA). The grafting fluorosilicone copolymer onto starch improves obviously their hydrophobic and thermal properties. Comparatively, VTMS‐starch@P(MMA/BA/3FMA) film performs higher water contact angle (107°) and thermal stability (350–430°C) than p(VTMS/12FMA)‐g‐starch film (72°, 250–420°C) due to the migration of fluorine‐containing group onto the surface of film during the film formation. Therefore, VTMS‐starch@P(MMA/BA/3FMA) shows much better protective performance in water‐resistance, and salt/freeze‐thaw resistance for stone samples. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41650.     

Preparation and properties of catalyzed polyimide/dicyanate semi‐interpenetrating networks for polymer gas membrane with suppressed CO2‐plasticization

The work presents an approach to reduce the plasticization of polymeric membranes caused by condensable gases, and particularly the effect of plasticization caused on polyimides by CO₂ at high pressure. A technical polyimide, Matrimid^®, was chosen as a reference of polyimide membrane and the approach applied consisted of incorporating reactive oligomers to have cross‐linkable mixed systems, which do not plasticize at high CO₂ pressure. Films of semi‐interpenetrating networks (semi‐IPNs) based on Matrimid^® and phenolphthalein dicyanate as cross‐linking monomer in ratios 90/10, 80/20, and 70/30, were prepared using a catalyst to lower the curing temperature from 280 to 180°C. Semi‐IPNs properties such as thermal stability, mechanical properties, glass transition temperatures, or density were measured to characterize the films and were correlated with the dicyanate monomer content. The CO₂ gas permeation behavior of the three semi‐IPNs was studied using a CO₂ feed pressure ranging from 1 to 30 atm. The gas separation properties were mainly explained attending to the density of the films, which depended on the dicyanate content used. In the three catalyzed semi‐IPNs, the CO₂ permeability coefficients remained almost constant all along the investigated range of CO₂ pressure while Matrimid^® treated at 180°C did show a clear tendency to plasticization over a critical feed pressure of about 17 bar. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Aqueous polyacrylate/poly(silicone‐co‐acrylate) emulsion coated fertilizers for slow nutrient‐release application

Waterborne polyacrylate/poly(silicone‐co‐acrylate) emulsions were synthesized to develop coated fertilizers. The effects of the n‐butyl acrylate (BA)/methyl methacrylate (MMA) ratio, vinyltriethoxysilane, and synthesis method on the water resistance, glass‐transition temperature, mechanical properties, and nutrient‐release profiles were investigated. The results show that miniemulsion polymerization with a BA/MMA ratio of 55:45 was the most suitable for slow nutrient‐release applications. Under these conditions, the preliminary solubility rate of the nutrient was about 3%, and the 30‐day cumulative nutrient release was 15% at 25°C. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40369.     

Study of the effect of natural rubber‐graft‐o‐aminophenol on the thermal stability and mechanical properties of nitrile rubber

The grafting copolymerization of natural rubber and o‐aminophenol was carried out by using two‐roll mill machine. The prepared grafted antioxidant, NR‐graft‐o‐AP, analyzed by using Infrared and ¹H‐NMR Spectroscopy techniques. The thermal stability, mechanical properties, and ultrasonic attenuation coefficient were evaluated for NBR vulcanizates containing the commercial antioxidant, PBN, and the prepared grafted antioxidant, NR‐graft‐o‐AP, and the control vulcanizate. Results of the thermal stability indicate that the prepared NR‐graft‐o‐AP can protect NBR vulcanizate against thermal treatment much better than the commercial antioxidant, PBN, and control mix, respectively. The prepared grafted antioxidant improves the mechanical properties of NBR vulcanizate. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Interpenetrating polymer networks based on poly(styrene‐co‐butylacrylate‐co‐hydroxyethyl methacrylate) and SiO2

Copolymer such as poly(styrene‐co‐butylacrylate‐co‐hydroxyethyl methacrylate) p (St‐BA‐HEMA) was prepared via free radical emulsion polymerization method. The resulting copolymer was converted to silicone secondary crosslinked interpenetrating polymer network (IPN) by condensation reaction with tetraethyl orthosilicate (TEOS). The obtained copolymers were characterized by using Fourier transform infrared spectroscopy (FTIR). Thermal properties of the copolymers were studied by using thermogravimetric analysis (TGA) and differential scanning calorimetry (DSC). Optical microscopy (OM) is used for studying the morphology, and then the effects of silicone concentrations, the reflux time, and composition on the phase morphology of P (St‐BA‐HEMA)‐SiO₂ IPNs were discussed. The broadening of the transition region was observed with the prolongation of the reflux time, and the tendency for aggregation of silicone on the surface was observed with Teflon as substrate plate. However, an optically transparent film was easily achieved at higher temperature due to the chemical crosslink and physical entanglement between the two phases of P (St‐BA‐HEMA)‐SiO₂. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Novel peroxide‐vulcanized NBR‐PAni.DBSA blends,part 2: Effects of conductive filler particles alignment

Dicumyl peroxide (DCP) vulcanized poly(butadiene‐co‐acrylonitrile)‐polyaniline dodecylbenzenesulfonate [NBR‐PAni.DBSA] blends were successfully prepared by using the practical thermomechanical mixing method. The effect of alignment of PAni.DBSA particles on the mechanical and electrical properties of vulcanized blends was studied (by passing the blends through a two roll‐mills). All vulcanized blends strained parallel to the flow direction when passed through the two roll‐mills had their electrical conductivities enhanced with increasing strain in tension. Good historical memory in term of the electrical conductivities during three cycles of straining (with 300 times of strain loading and unloading motion for each cycle) was observed for all vulcanized blends (99% retention of original value before straining). These vulcanized blends also showed better mechanical properties (i.e., higher tensile strength and tear strength) than the ones strained perpendicularly to the flow direction. With the ideal mechanical properties and reversible electrical behavior, this type of blend can potentially emerge as a new class of flexible smart material. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2012     

Morphologies and dynamic mechanical properties of core‐shell emulsifier‐free latexes and their copolymers for P(BA/MMA)/P(MMA/BA) and P(BA/MMA)/PSt systems in the presence of AHPS

Different poly(methyl methacrylate/n‐butyl acrylate)/poly(n‐butyl acrylate/methyl methacrylate) [P(BA/MMA)/P(MMA/BA)] and poly(n‐butyl acrylate/methyl methacrylate)/polystyrene [P(BA/MMA)/PSt] core‐shell structured latexes were prepared by emulsifier‐free emulsion polymerization in the presence of hydrophilic monomer 3‐allyloxy‐2‐hydroxyl‐propanesulfonic salt (AHPS). The particle morphologies of the final latexes and dynamic mechanical properties of the copolymers from final latexes were investigated in detail. With the addition of AHPS, a latex of stable and high‐solid content (60 wt %) was prepared. The diameters of the latex particles are ～0.26 μm for the P(BA/MMA)/P(MMA/BA) system and 0.22–0.24 μm for the P(BA/MMA)/PSt system. All copolymers from the final latexes are two‐phase structure polymers, shown as two glass transition temperatures (T_gs) on dynamic mechanical analysis spectra. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 3078–3084, 2002     

Comparison of viscoelastic properties of polydimethylsiloxane/poly(2‐hydroxyethyl methacrylate) IPNs with their physical blends

Interpenetrating polymer networks (IPNs) of polydimethylsiloxane (PDMS) and poly(2‐hydroxyethyl methacrylate) (PHEMA) were prepared by sequential method. The dynamic mechanical parameters of obtained IPNs and their variations with the structural composition were evaluated. The results for the IPNs were compared with corresponding physically blended systems. The tensile properties and damping factor (tan δ) were assessed by stress–strain measurement and dynamic mechanical thermal analysis (DMTA), respectively. The glass–rubber transition temperature (T_g) was assessed by DMTA and differential scanning calorimetry (DSC). The results showed higher tensile strength and elongation at break for IPNs than those for physical blends. The shifts of T_g for that two components that make up the IPNs were greater than those for corresponding blends. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 3480–3485, 2002     

Nitrile rubber/hindered phenol exterminated hyperbranched polyester materials with improved damping and mechanical performance

Hindered phenol exterminated hyperbranched polyester (mHBP) is fabricated by esterification reaction. The mHBP is introduced into nitrile rubber (NBR) to prepare NBR/mHBP blends. Structure, damping and mechanical properties of NBR/mHBP blends are investigated by Fourier transform infrared spectroscopy (FTIR), ¹H‐NMR, dynamic mechanical thermal analyzer (DMTA), and tensile tester. FTIR spectra of the blends illustrate the intermolecular hydrogen bonding between the NBR and mHBP, contributing to the improvement of damping and mechanical properties. The results indicate that, with the increasing mHBP content, the T_g of the blends shifted to a higher temperature with a broadening temperature range and improved mechanical properties, showing an application in adjusting the T_g and temperature range without decreasing of loss factor. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42605.     

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