Use of zinc‐neutralized ethylene/methacrylic acid copolymer ionomers as blend compatibilizers for nylon 6 and low‐density polyethylene

The effect of the composition on the morphologies and properties of uncompatibilized and compatibilized blends of nylon 6 and low‐density polyethylene were studied over a wide range of weight fractions. The uncompatibilized blends had substantially reduced mechanical properties after mixing, and this was almost certainly due to poor interfacial adhesion between the two polymers. The addition of a zinc‐neutralized poly(ethylene‐co‐methacrylic acid) ionomer (Surlyn® 9020) as a compatibilizer improved the mechanical properties in comparison with those of the material blended without the compatibilizer. The clearest evidence of this improvement came from dynamic mechanical studies; for selected blends with high polyethylene contents, the drop in the modulus corresponding to the transition of a solid to a melt occurred at higher temperatures with the added compatibilizer. This improvement in the properties was accompanied by a reduction in the dispersed‐phase size due to the interaction between the ionic part of the ionomer and the amide groups of nylon 6, especially when nylon 6 was the dispersed phase of the blend. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 89: 620–629, 2003     

Effect of the high‐density polyethylene melt index on the microcellular foaming of high‐density polyethylene/polypropylene blends

The effect of high‐density polyethylene (HDPE)/polypropylene (PP) blending on the crystallinity as a function of the HDPE melt index was studied. The melting temperature and total amount of crystallinity in the HDPE/PP blends were lower than those of the pure polymers, regardless of the blend composition and melt index. The effects of the melt index, blending, and foaming conditions (foaming temperature and foaming time) on the void fractions of HDPEs of various melt indices and HDPE/PP blends were also investigated. The void fraction was strongly dependent on the foaming time, foaming temperature, and blend composition as well as the melt index of HDPE. The void fraction of the foamed 30:70 HDPE/PP blend was always higher than that of the foamed 50:50 HDPE/PP blend, regardless of the melt index. The microcellular structure could be greatly improved with a suitable ratio of HDPE to PP and with foaming above the melting temperature for long enough; however, using high‐melt‐index HDPE in the HDPE/PP blends had a deleterious effect on both the void fraction and cell morphology of the blends. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 93: 364–371, 2004     

Thermoplastic vulcanizates based on epoxidized natural rubber/polypropylene blends: Effect of compatibilizers and reactive blending

Epoxidized natural rubber (ENR) was prepared using the performic epoxidation method. TPVs based on ENR/PP blends were later prepared by melt‐mixing processes via dynamic vulcanization. The effects of blend ratios of ENR/PP, types of compatibilizers, and reactive blending were investigated. Phenolic modified polypropylene (Ph‐PP) and graft copolymer of maleic anhydride on polypropylene molecules (PP‐g‐MA) were prepared and used as blend compatibilizers and reactive blending components of ENR/Ph‐PP and ENR/PP‐g‐MA blends. It was found that the mixing torque, apparent shear stress and apparent shear viscosity increased with increasing levels of ENR. This is attributed to the higher viscosity of the pure ENR than that of the pure PP. Furthermore, there was a higher compatibilizing effect because of the chemical interaction between the polar groups in ENR and PP‐g‐MA or Ph‐PP. Mixing torque, shear flow properties (i.e., shear stress and shear viscosity) and mechanical properties (i.e., tensile strength, elongation at break, and hardness) of the TPVs prepared by reactive blending of ENR/Ph‐PP and ENR/PP‐g‐MA were lower than that of the samples without a compatibilizer. However, the TPVs prepared using Ph‐PP and PP‐g‐MA as compatibilizers exhibited higher values. We observed that the TPVs prepared from ENR/PP with Ph‐PP as a compatibilizer gave the highest rheological and mechanical properties, while the reactive blending of ENR/PP exhibited the lowest values. Trend of the properties corresponds to the morphology of the TPVs. That is, the TPV with Ph‐PP as a blend compatibilizer showed the smallest rubber particles dispersed in the PP matrix, while the reactive blending of ENR/PP‐g‐MA showed the largest particles. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 100: 4729–4740, 2006     

Thermoplastic elastomers based on recycled high‐density polyethylene,ethylene–propylene–diene monomer rubber,and ground tire rubber

High‐performance thermoplastic elastomers (TPEs), based on recycled high‐density polyethylene (HDPE^R), olefinic type ethylene–propylene–diene monomer rubber (EPDM), and ground tire rubber (GTR) treated with bitumen, were prepared by using dynamic vulcanization technology, and their structure–property relationships were investigated. It was established that special pretreatment of GTR by bitumen confers outstanding mechanical properties on the resulting TPEs. TPEs, containing GTR pretreated by bitumen, exhibit thermal behavior similar to that of the HDPE^R/EPDM basic blend in the temperature region up to about 340°C. Rheological measurements showed that bitumen acts as an effective plasticizer for the GTR‐containing TPEs. SEM, DSC, and DMTA results revealed improved adhesion between the particles of GTR treated by bitumen and the surrounding thermoplastic matrix, compared to that of the untreated GTR particles. It was concluded that bitumen acts as an effective devulcanizing agent in the GTR treatment stage. In the following steps of TPE production, bitumen acts simultaneously as a curing agent for the rubber components (EPDM/GTR) and as a compatibilizer for the blend components. GTR‐containing TPEs, prepared by extrusion technology, were reprocessed (by passing through the extruder six times) without any observable changes in their tensile properties, thermal stability, and melt viscosity. © 2004 Wiley Periodicals, Inc. J Appl Polym Sci 95: 659–671, 2005     

Dynamic mechanical behavior of high‐density polyethylene/ethylene vinyl acetate copolymer blends: The effects of the blend ratio,reactive compatibilization,and dynamic vulcanization

The effects of the blend ratio, reactive compatibilization, and dynamic vulcanization on the dynamic mechanical properties of high‐density polyethylene (HDPE)/ethylene vinyl acetate (EVA) blends have been analyzed at different temperatures. The storage modulus of the blend decreases with an increase in the EVA content. The loss factor curve shows two peaks, corresponding to the transitions of HDPE and EVA, indicating the incompatibility of the blend system. Attempts have been made to correlate the observed viscoelastic properties of the blends with the blend morphology. Various composite models have been used to predict the dynamic mechanical data. The experimental values are close to those of the Halpin–Tsai model above 50 wt % EVA and close to those of the Coran model up to 50 wt % EVA in the blend. For the Takayanagi model, the theoretical value is in good agreement with the experimental value for a 70/30 HDPE/EVA blend. The area under the loss modulus/temperature curve (LA) has been analyzed with the integration method from the experimental curve and has been compared with that obtained from group contribution analysis. The LA values calculated with group contribution analysis are lower than those calculated with the integration method. The addition of a maleic‐modified polyethylene compatibilizer increases the storage modulus, loss modulus, and loss factor values of the system, and this is due to the finer dispersion of the EVA domains in the HDPE matrix upon compatibilization. For 70/30 and 50/50 blends, the addition of a maleic‐modified polyethylene compatibilizer shifts the relaxation temperature of both HDPE and EVA to a lower temperature, and this indicates increased interdiffusion of the two phases at the interface upon compatibilization. However, for a 30/70 HDPE/EVA blend, the addition of a compatibilizer does not change the relaxation temperature, and this may be due to the cocontinuous morphology of the blends. The dynamic vulcanization of the EVA phase with dicumyl peroxide results in an increase in both the storage and loss moduli of the blends. A significant increase in the relaxation temperature of EVA and a broadening of the relaxation peaks occur during dynamic vulcanization, and this indicates the increased interaction between the two phases. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 87: 2083–2099, 2003     

Studies on blends of high‐density polyethylene and polypropylene produced by oscillating shear stress field

Tensile strength and morphology of blends of high‐density polyethylene (HDPE) and polypropylene (PP) obtained by oscillating packing injection molding were investigated via Universal Testing Machine, DSC, and SAXS. Tensile strength is greatly enhanced from 24.5 MPa to more than 90 MPa for pure HDPE and for blends with PP content less than 10 wt %. There exists a sharp decrease of tensile strength when PP content is more than 10 wt %. The shear‐induced morphologies with core in the center, oriented zone surrounding the core and skin layer are observed in the cross‐section areas of the samples. Interestingly, a sharp decrease of oriented zone is seen when PP content is more than 10 wt %, associated with the sharp decrease of tensile strength. DSC result shows double melting peaks with a high‐temperature melting peak that is not present in the endotherm obtained from the central core and obtained from the samples by static packing injection molding, which indicates the existence of shish‐kebab structure in the oriented zone. However, there is no difference of crystallinity between the samples by oscillating and by static packing injection molding. SAXS was used to analyze the complicated morphologies induced by shear stress, and results show that the crystal thickness could be greatly increased under shear stress. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 58–63, 2002     

Mechanical properties and blend compatibility of natural rubber –chlorosulfonated polyethylene blends

Natural rubber (NR) was blended with chlorosulfonated polyethylene (CSM) with various formulation and blend ratios (NR/CSM: 80/20 –20/80, wt/wt). Rubber blends were prepared by using a two‐roll mill and vulcanized in a compression mold to obtain the 2 mm‐thick sheets. Tensile properties, tear resistance, thermal aging resistance, ozone resistance, and oil resistance were determined according to ASTM. Compatible NR/CSM blends are derived from certain blends containing 20–30% CSM without adding any compatibilizing agent. Tensile and tear strength of NR‐rich blends for certain formulations show positive deviation from the rule of mixture. Thermal aging resistance depends on formulation and blend ratio, while ozone and oil resistance of the blends increase with CSM content. Homogenizing agents used were Stuktol®60NS and Epoxyprene®25. Stuktol®60NS tends to decrease the mechanical properties of the blends and shows no significant effect on blend morphology. Addition of 5–10 phr of epoxidized natural rubber (ENR, Epoxyprene® 25) increases tensile strength, thermal aging resistance, and ozone resistance of the blends. It is found that ENR acts as a compatibilizer of the NR/CSM blends by decreasing both CSM particle size diameter and α transition temperature of CSM. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 99: 127–140, 2006     

Thermal and mechanical properties of linear low‐density polyethylene/low‐density polyethylene/wax ternary blends

The thermal and mechanical properties of uncrosslinked three‐component blends of linear low‐density polyethylene (LLDPE), low‐density polyethylene (LDPE), and a hard, paraffinic Fischer–Tropsch wax were investigated. A decrease in the total crystallinity with an increase in both LDPE and wax contents was observed. It was also observed that experimental enthalpy values of LLDPE in the blends were generally higher than the theoretically expected values, whereas in the case of LDPE the theoretically expected values were higher than the experimental values. In the presence of higher wax content there was a good correlation between experimental and theoretically expected enthalpy values. The DSC results showed changes in peak temperature of melting, as well as peak width, with changing blend composition. Most of these changes are explained in terms of the preferred cocrystallization of wax with LLDPE. Young's modulus, yield stress, and stress at break decreased with increasing LDPE content, whereas elongation at yield increased. This is in line with the decreasing crystallinity and increasing amorphous content expected with increasing LDPE content. Deviations from this behavior for samples containing 10% wax and relatively low LDPE contents are explained in terms of lower tie chain fractions. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 96: 1748–1755, 2005     

Novel dynamic vulcanization of polyethylene and ozonolysed natural rubber blends: Effect of curing system and blending ratio

Dynamic vulcanization was studied in terms of the change in α‐relaxation temperatures of the LDPE matrix, morphology, and mechanical properties of LDPE/ozonolysed NR blends which were vulcanized at various blend ratios and with different curing systems, i.e., peroxide and sulfur systems. The ozonolysed NR with M _w = 8.30 × 10⁵ g mol⁻¹ and M _n = 2.62 × 10⁵ g mol⁻¹, prepared by the in situ ozonolysis reaction of natural rubber latex, was used in this study. The significant change in the α‐relaxation temperature of LDPE in the LDPE/ozonolysed NR, dynamically vulcanized using the sulfur system, suggested that sulfur vulcanization of the blend gave a higher degree of crosslink density than using peroxide and corresponded with the improved damping property and homogenous phase morphology. However, the peroxide cured blends of LDPE/ozonolyzed NR gave more improvement of tensile strength and elongation at break than the sulfur cured system. Furthermore, the mechanical properties of tensile strength, elongation at break, and damping were improved by increasing the ozonolyzed natural rubber content in both DCP and sulfur cured blends. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Poly(ethylene‐co‐methacrylic acid)–lithium ionomer as a compatibilizer for poly(ethylene terephthalate)/linear low‐density polyethylene blends

Poly(ethylene terephthalate) (PET)/linear low‐density polyethylene (LLDPE) blends (75/25), with contents of poly(ethylene‐co‐methacrylic acid) partially neutralized with lithium (PEMA–Li) that were systematically changed from 0 to 45% relative to the LLDPE, were obtained by direct injection molding in an attempt to (1) ameliorate the performance of the binary blend and (2) find the best compatibilizer content. PEMA–Li did not modify the PET or LLDPE amorphous‐phase compositions or the crystalline content of PET. However, PEMA–Li did lead to a nucleation effect and to the presence of a second smaller and less perfect crystalline structure. PET induced a fractional crystallization in LLDPE that remained in the presence of PEMA–Li and reduced the crystallinity of LLDPE. The ternary blends showed two similar dispersed LLDPE and PEMA–Li phases with small subparticles, probably PET, inside. The compatibilizing effect of PEMA–Li was clearly shown by the impressive increase in the break strain, along with only small decreases in the modulus of elasticity and in the tensile strength. With respect to the recycling possibilities of LLDPE, a ternary blend with the addition of 22.5% PEMA–Li, which led to very slight modulus and yield stress decreases with respect to the binary blend and a break strain increase of 480%, appeared to be the most attractive. However, the highest property improvement appeared with the addition of 37.5% PEMA–Li, which led to elasticity modulus and tensile strength decreases of only 9%, along with a very high break strain increase (760%). © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 87: 1322–1328, 2003     

High‐density polyethylene/ultrahigh‐molecular‐weight polyethylene blend. I. The processing,thermal, and mechanical properties

Various blend ratios of high‐density polyethylene (HDPE) and ultrahigh‐molecular‐weight polyethylene (UHMWPE) were prepared with the objective of determining their suitability as biomaterials. Although the presence of HDPE in the blends enabled melt processing, the presence of UHMWPE helped to improve the toughness of the resulting blends. The processability of the blends was investigated with the Brabender torque, which was used as an indication of the optimum blend conditions. The blends were characterized with differential scanning calorimetry. The mechanical tests performed on the blends included tensile, flexural, and impact tests. A 50:50 (w/w) blend yielded optimum properties in terms of the processability and mechanical properties. The tensile property of the 50:50 blend was intermediate between those of HDPE and UHMWPE, but the strain at break increased 200% in comparison with that of both neat resins. The energy at break of the 50:50 blend revealed an improvement in the toughness. The fracture mechanism was also investigated with scanning electron microscopy. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 97: 413–425, 2005     

Thermoplastic vulcanizates based on poly(methyl methacrylate)/epoxidized natural rubber blends: Mechanical,thermal, and morphological properties

Epoxidized natural rubbers (ENRs) with epoxide levels of 10, 20, 30, 40 and 50 mol % were prepared. The ENRs were later used to prepare thermoplastic vulcanizates (TPVs) by blending them with poly(methyl methacrylate) (PMMA) using various formulations. Dynamic vulcanization, using sulfur as a vulcanizing agent, was performed during the mixing process. The mixing torque increased as the ENR contents and epoxide molar percentage increased. This was because of an increasing chemical interaction between the polar groups of the blend components, particularly at the interface between the elastomeric and thermoplastic phases. The ultimate tensile strength of the TPVs with ENR‐20 was high because of strain‐induced crystallization. ENRs with epoxide levels >30 mol % exhibited an increase of tensile strength because of increasing levels of chemical interaction between the molecules and the different phases. The hardness of the TPVs also increased with increased epoxide levels but decreased with increased contents of ENRs. Two morphology phases with small domains of vulcanized ENR particles dispersed in the PMMA matrix were observed from scanning electron microscopy micrographs. The TPVs based on ENR‐20 and ENR‐50 showed smaller dispersed rubber domains than those of the other types of ENRs. Furthermore, the size of the vulcanized rubber domain decreased with increasing amounts of PMMA in the blends. The decomposition temperature of the TPVs also increased as both the levels of ENRs in the blends and the epoxide molar percentage increased. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 98: 1251–1261, 2005     

Influence of compatibilizers on the rheological,mechanical, and morphological properties of epoxidized natural rubber/polypropylene thermoplastic vulcanizates

In polymeric materials combining desirable properties, compatibility between constituent components of incompatible blends is necessary. The influence of two types of blend compatibilizers, a graft copolymer of maleic anhydride and polypropylene (PP) and phenolic‐modified PP, on the rheological, mechanical, and morphological properties of epoxidized natural rubber/PP thermoplastic vulcanizates was investigated at varied concentrations. All properties improved in a range of loading levels of compatibilizers at 0–7.5 wt % of PP. This was attributed to a chemical interaction between the different phases caused by the functionalized compatibilizers. Increasing chemical interaction between interfaces improved the interfacial tension and led to a microscale size of the dispersion. A decreasing trend in the properties was observed at compatibilizer levels higher than 7.5 wt % of PP because of segregation, which led to a third blend component dispersed in the PP matrix. The compatibilizers behaved as lubricants in the polymer melt flow. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci, 2008     

Polyamide‐reinforced ethylene–propylene–diene rubber compatibilized with chlorinated polyethylene

Vulcanizates of blends of ethylene–propylene–diene rubber and polyamide copolymers were prepared by reactive compatibilization. A reactive route was employed for compatibilizing these blends with the addition of chlorinated polyethylene (CPE). The influence of the compatibilizers, crosslinking agents, blend compositions, and addition modes of the compatibilizers on the mechanical properties of the blends was investigated. The morphologies of the blends were determined with scanning electron microscopy. The addition of CPE was found to reduce the particle size of the dispersed phase remarkably. The stability of the blends with compatibilizers was measured by high‐temperature thermal aging. The mechanical properties were examined by stress–strain measurements and dynamic mechanical thermal measurements; the addition of polyamide copolymers caused significant improvements in the tensile properties of these blends.© 2003 Wiley Periodicals, Inc. J Appl Polym Sci 89: 1727–1736, 2003     

Characterization of the free volume in high‐impact polystyrene/polypropylene and high‐impact polystyrene/high‐density polyethylene blends probed by positron annihilation spectroscopy

The free‐volume properties of high‐impact polystyrene (HIPS)/polypropylene (PP) and HIPS/high‐density polyethylene (HDPE) blends were investigated by means of positron annihilation lifetime spectroscopy (PALS). The measured results show that the free‐volume holes in the semicrystalline polymers, such as PP and HDPE, were not large enough to accommodate the branched chains and the end groups of the macromolecular chains in HIPS to produce favorable interactions between the semicrystalline polymers and the HIPS polymer in these blends; thus immiscible blends were formed. The weak interaction between two dissimilar polymer molecules only took place in the regions between two amorphous phases. In addition, the observed negative deviations of the longest lifetime intensity and the free‐volume fraction were attributed to the influence of the interfacial polarization during PALS measurement. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 90: 1507–1514, 2003     

Mechanical and thermal properties of high‐density polyethylene toughened with glass beads

Glass beads were used to improve the mechanical and thermal properties of high‐density polyethylene (HDPE). HDPE/glass‐bead blends were prepared in a Brabender‐like apparatus, and this was followed by press molding. Static tensile measurements showed that the modulus of the HDPE/glass‐bead blends increased considerably with increasing glass‐bead content, whereas the yield stress remained roughly unchanged at first and then decreased slowly with increasing glass‐bead content. Izod impact tests at room temperature revealed that the impact strength changed very slowly with increasing glass‐bead content up to a critical value; thereafter, it increased sharply with increasing glass‐bead content. That is, the Izod impact strength of the blends underwent a sharp transition with increasing glass‐bead content. It was calculated that the critical interparticle distance for the HDPE/glass‐bead blends at room temperature (25°C) was 2.5 μm. Scanning electron microscopy observations indicated that the high impact strength of the HDPE/glass‐bead blends resulted from the deformation of the HDPE matrix. Dynamic mechanical analyses and thermogravimetric measurements implied that the heat resistance and heat stability of the blends tended to increase considerably with increasing glass‐bead content. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 89: 2102–2107, 2003     

Melt strength of linear low‐density polyethylene/low‐density polyethylene blends

Linear low‐density polyethylenes and low‐density polyethylenes of various compositions were melt‐blended with a batch mixer. The blends were characterized by their melt strengths and other rheological properties. A simple method for measuring melt strength is presented. The melt strength of a blend may vary according to the additive rule or deviate from the additive rule by showing a synergistic or antagonistic effect. This article reports our investigation of the parameters controlling variations of the melt strength of a blend. The reciprocal of the melt strength of a blend correlates well with the reciprocal of the zero‐shear viscosity and the reciprocal of the relaxation time of the melt. An empirical equation relating the maximum increment (or decrement) of the melt strength to the melt indices of the blend components is proposed. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 85: 1408–1418, 2002     

Rheological behavior and mechanical properties of high‐density polyethylene blends with different molecular weights

The dynamic rheological and mechanical properties of the binary blends of two conventional high‐density polyethylenes [HDPEs; low molecular weight (LMW) and high molecular weight (HMW)] with distinct different weight‐average molecular weights were studied. The rheological results show that the rheological behavior of the blends departed from classical linear viscoelastic theory because of the polydispersity of the HDPEs that we used. Plots of the logarithm of the zero shear viscosity fitted by the Cross model versus the blend composition, Cole–Cole plots, Han curves, and master curves of the storage and loss moduli indicated the LMW/HMW blends of different compositions were miscible in the melt state. The tensile yield strength of the blends generally followed the linear additivity rule, whereas the elongation at break and impact strength were lower than those predicted by linear additivity; this suggested the incompatibility of the blends in solid state. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2010     

Correlation between the morphology and dynamic mechanical properties of ethylene vinyl acetate/linear low‐density polyethylene blends: Effects of the blend ratio and compatibilization

The effects of the blend composition and compatibilization on the morphology of linear low‐density polyethylene (LLDPE)/ethylene vinyl acetate (EVA) blends were studied. The blends showed dispersed/matrix and cocontinuous phase morphologies that depended on the composition. The blends had a cocontinuous morphology at an EVA concentration of 40–60%. The addition of the compatibilizer first decreased the domain size of the dispersed phase, which then leveled off. Two types of compatibilizers were added to the polymer/polymer interface: linear low‐density polyethylene‐g‐maleic anhydride and LLDPE‐g phenolic resin. Noolandi's theory was in agreement with the experimental data. The conformation of the compatibilizer at the blend interface could be predicted by the calculation of the area occupied by the compatibilizer molecule at the interface. The effects of the blend ratio and compatibilization on the dynamic mechanical properties of the blends were analyzed from ?60°C to +35°C. The experiments were performed over a series of frequencies. The area under the curve of the loss modulus versus the temperature was higher than the values obtained by group contribution analysis. The loss tangent curve showed a peak corresponding to the glass transition of EVA, indicating the incompatibility of the blend system. The damping characteristics of the blends increased with increasing EVA content because of the decrease in the crystalline volume of the system. Attempts were made to correlate the observed viscoelastic properties of the blends with the morphology. Various composite models were used to model the dynamic mechanical data. Compatibilization increased the storage modulus of the system because of the fine dispersion of EVA domains in the LLDPE matrix, which provided increased interfacial interaction. Better compatibilization was effected at a 0.5–1% loading of the compatibilizer. This was in full agreement with the dynamic mechanical spectroscopy data. © 2006 Wiley Periodicals, Inc. J Appl Polym Sci 100: 4526–4538, 2006     

Rheological and thermal properties of single‐site polyethylene blends

Branched polyethylenes, low‐density polyethylenes (LDPE1 and LDPE2) or long‐chain‐branched very low density polyethylenes (VLDPE2), were blended with very low density polyethylenes containing short branches (VLDPE1 and VLDPE3). The rheological and thermal measurements of the pure copolymers and their blends (VLDPE1–LDPE1, VLDPE1–LDPE2, VLDPE1–VLDPE2, and VLDPE2–VLDPE3) were taken by controlled stress rheometry and differential scanning calorimetry, respectively. The shear‐thinning effect became stronger with increasing long‐chain‐branched polymer compositions when it was correlated with the flow behavior index, and the extent of shear thinning was different for each blend set. Stronger shear thinning and a linear composition dependence of the zero‐shear viscosity were observed for the VLDPE1–LDPE1 and VLDPE1–LDPE2 blends. These blends followed the log additivity rule, and this indicated that they were miscible in the melt at all compositions. In contrast, a deviation from the log additivity rule was observed for the VLDPE1–VLDPE2 blend compositions with 50% or less VLDPE2 and for the VLDPE3–VLDPE2 blends with 50% or more VLDPE2. The thermal properties of the blends were consistent with the rheological properties. VLDPE1–LDPE1 and VLDPE1–LDPE2 showed that these blends were characteristic of a single‐component system at all compositions, whereas the phase separation (immiscibility) was detected only for VLDPE1–VLDPE2 blends with 50% or less VLDPE2 and for VLDPE3–VLDPE2 blends with 50% or more VLDPE2. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 95: 1549–1557, 2005