Miscibility and phase behavior in thermosetting blends of polybenzoxazine and poly(ethylene oxide)

Thermosetting polymer blends composed of polybenzoxazine (PBA-a) and poly(ethylene oxide) (PEO) were prepared via in situ curing reaction of benzoxazine (BA-a) in the presence of PEO, which started from the initially homogeneous mixtures of BA-a and PEO. Before curing, the BA-a/PEO blends displayed the single and composition-dependant glass transition temperatures (T_g's) in the entire blend composition, and the equilibrium melting point depression was also observed in the blends. It is judged that the BA-a/PEO blends are completely miscible. The miscibility was mainly ascribed to the contribution of entropy to mixing free energy since the molecular weight of BA-a is rather low. However, phase separation occurred after curing reaction at the elevated temperature, which was confirmed by differential scanning calorimetry (DSC) and scanning electronic microscopy (SEM). It was expected that the PBA-a/PEO blends would be miscible since PBA-a possesses a great number of phenolic hydroxyls in the molecular backbone, which are potential to form the intermolecular hydrogen bonding interactions with oxygen atoms of PEO and thus would fulfill the miscibility of the blends. To interpret the experimental results, we investigated the variable temperature Fourier transform infrared spectroscopy (FTIR) of the blends via model compound. The FTIR results indicate that the phenolic hydroxyl groups could not form the efficient intermolecular hydrogen bonding interactions at the elevated temperatures (e.g. the curing temperatures), i.e. the phenolic hydroxyl groups existed mainly in the non-associated form in the system. Therefore, the decrease of the mixing entropy still dominates the phase behavior of thermosetting blends at the elevated temperature.     

Blends of poly(ethylene oxide) and poly(4-vinylphenol-co-2-hydroxyethyl methacrylate): thermal analysis, morphological behaviour and specific interactions

DSC and optical microscopy were used to determine the miscibility and crystallinity of blends of poly(ethylene oxide) (PEO) with poly(4-vinylphenol-co-2-hydroxyethyl methacrylate) (PVPh-HEM). A single glass transition temperature was observed for all blends, indicating miscibility. A progressive decrease in the degree of crystallinity and in the size of the PEO spherullites is observed, as PVPh-HEM is added. FTIR was used to probe the intermolecular specific interactions of the blends and the miscibility of the blend is mainly attributed to PVPh-HEM/PEO intermolecular interactions via hydrogen bonding.     

Inorganic-organic interpenetrating polymer networks involving polyhedral oligomeric silsesquioxane and poly(ethylene oxide)

A novel organic-inorganic interpenetrating polymer network (IPN) was prepared via in situ crosslinking between octa(propylglycidyl ether) polyhedral oligomeric silsesquioxane (OpePOSS) and 2,2-bis(4-hydroxyphenyl)propane in the presence of poly(ethylene oxide) (PEO). The miscibility and intermolecular specific interactions of the IPNs were investigated by means of differential scanning calorimetry (DSC), transmission electron microscopy (TEM) and Fourier transform infrared (FTIR) spectroscopy. In view of the results of calorimetric analysis and morphological observation, it is judged that the components of the organic-inorganic IPNs are fully miscible. The FTIR spectroscopy shows that there are inter-component hydrogen bonding interactions between the POSS network and PEO. The measurements of static contact angle show that the hydrophilicity (and/or the surface free energy) of the organic-inorganic IPNs increased with the addition of the miscible and water-soluble polymer (i.e., PEO). Thermogravimetric analysis (TGA) shows that the thermal stability of the IPNs was quite dependent on the mass ratios of the POSS network to PEO.     

Kraft lignin/poly(ethylene oxide) blends: Effect of lignin structure on miscibility and hydrogen bonding

Blends of poly(ethylene oxide) (PEO) with softwood kraft lignin (SKL) were prepared by thermal blending. The miscibility behavior and hydrogen bonding of the blends were investigated by differential scanning calorimetry (DSC) and Fourier transform infrared (FTIR) spectroscopy. The experimental results indicate that PEO was miscible with SKL, as shown by the existence of a single glass‐transition temperature over the entire composition range by DSC. In addition, a negative polymer–polymer interaction energy density was calculated on the basis of the melting point depression of PEO. The formation of strong intermolecular hydrogen bonding was detected by FTIR analysis. A comparison of the results obtained for the SKL/PEO blend system with those previously observed for a hardwood kraft lignin/PEO system revealed the existence of stronger hydrogen bonding within the SKL/PEO blends but weaker overall intermolecular interactions between components; this suggested that more than just hydrogen bonding was involved in the determination of the blend behavior in the kraft lignin/PEO blends. © 2005 Wiley Periodicals, Inc. J Appl Polym Sci 98: 1437–1444, 2005     

Miscibility and intermolecular specific interactions in blends of poly(hydroxyether of bisphenol A) and poly(4-vinyl pyridine)

The blends of poly(hydroxyether of bisphenol A) (phenoxy) with poly(4-vinyl pyridine) (P4VPy) were investigated by differential scanning calorimetry (DSC), Fourier transform infrared spectroscopy (FTIR) and high-resolution solid-state nuclear magnetic resonance (NMR) spectroscopy. The single, composition-dependent glass transition temperature (T_g) was observed for each blend, indicating that the system is completely miscible. The sigmoid T_g-composition relationship is characteristic of the presence of the strong intermolecular specific interactions in the blend system. FTIR studies revealed that there was intermolecular hydrogen bonding in the blends and the intermolecular hydrogen bonding between the pendant hydroxyl groups of phenoxy and nitrogen atoms of pyridine ring is much stronger than that of self-association in phenoxy. To examine the miscibility of the system at the molecular level, the high resolution ¹³C cross-polarization (CP)/magic angle spinning (MAS) together with the high-power dipolar decoupling (DD) NMR technique was employed. Upon adding P4VPy to the system, the chemical shift of the hydroxyl-substituted methylene carbon resonance of phenoxy was observed to shift downfield in the ¹³C CP/MAS spectra. The proton spin-lattice relaxation time T₁(H) and the proton spin-lattice relaxation time in the rotating frame T_1ρ(H) were measured as a function of the blend composition. In light of the proton spin-lattice relaxation parameters, it is concluded that the phenoxy and P4VPy chains are intimately mixed on the scale of 20-30 Å.     

Poly(ethylene oxide) and its blends with sodium alginate

A series of blends based on poly(ethylene oxide) (PEO) and sodium alginate (NaAlg) were prepared by solution casting method. The blends thus obtained were characterized by using Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), tensile strength test, contact angle measurements and atomic force microscopy (AFM). FT-IR studies indicate that there are the hydrogen bonding interactions due to the ether oxygen of PEO and the hydroxyl groups of NaAlg. The thermal stability of the blends was slightly affected with increasing NaAlg content. DSC results showed that both melting point and crystallinity depend on the composition of the blends. Mechanical properties of the blend films were improved compared to those of homopolymers. Surface free energy components of the blend films were calculated from contact angle data of various liquids by using Van Oss-Good methodology. It was found that the surfaces both of the blends are enriched in low surface free energy component, i.e. NaAlg. This conclusion was further confirmed by the AFM images observation of the surface morphology of these blends.     

Miscibility and phase behavior in blends of phenolphthalein poly(ether sulfone) and poly(hydroxyether of bisphenol A)

Miscibility and phase behavior in the blends of phenolphthalein poly(ether sulfone) (PES-C) with poly(hydroxyether of bisphenol A) (PH) were investigated by means of differential scanning calorimetry (DSC), high resolution solid state nuclear magnetic resonance spectroscopy (NMR) and Fourier transform infrared spectroscopy (FTIR). It was found that the homogeneity of the as-prepared blends depended on the solvents used; N,N-dimethylformamide (DMF) provided the segmental mixing for PH and PES-C, which is confirmed by the behavior of single, composition-dependent glass transition temperatures (T_g's). To examine the homogeneity of the blends at the molecular level, the proton spin-lattice relaxation times in the rotating frame T_1ρ(H) were measured via ¹³C CP/MAS NMR spectroscopy as a function of blend composition. In view of the T_1ρ(H) values, it is concluded that the PH and PES-C chains are intimately mixed on the scale of 20-30 Å. FTIR studies indicate that there were the intermolecular specific interactions in this blends, involved with the hydrogen-bonding between the hydroxyls of PH and the carbonyls of PES-C, and the strength of the intermolecular hydrogen bonding is weaker than that of PH self-association. At higher temperature, the PH/PES-C blends underwent phase separation. By means of thermal analysis, the phase boundaries of the blends were determined, and the system displayed the lower critical solution temperature behavior. Thermogravity analysis (TGA) showed that the blends exhibited the improved thermal stability, which increases with increasing PES-C content.     

Influence of intramolecular specific interactions on phase behavior of epoxy resin and poly(ε-caprolactone) blends cured with aromatic amines

Two aromatic amines were used as the curing agents to prepare the thermosetting blends of epoxy and poly(ε-caprolactone) (PCL). When cured with 4,4′-methylenebis(2-chloroaniline) (MOCA), the thermosetting blends are miscible in the amorphous state in the entire composition, which was evidenced by the behavior of single, and composition-dependent glass transition temperatures (T_g's) in terms of thermal analysis. Fourier transform infrared spectroscopy (FTIR) showed that there are the intermolecular specific interactions (viz. hydrogen bonding) between the component polymers. However, the 4,4′-diaminodiphenylsulfone (DDS)-cured epoxy forms the immiscible blends with PCL. The blends displayed a typical reaction-induced phase separation morphology. The phase behavior seems to be more than the expected since it was ever proposed that there would be the intermolecular specific interactions between amine-cured epoxy and PCL, which would fulfill the miscibility of the systems. To interpret the phase behavior, we investigated that the miscibility and intermolecular specific interactions in the blends of model compounds and linear homologues of epoxy with PCL. It was observed that in MOCA-cured blends there were much stronger intermolecular specific interactions than in DDS-cured counterparts. The weaker intermolecular specific interactions between DDS-cured epoxy and PCL resulted from the formation of the intramolecular hydrogen bonding interactions within DDS-crosslinked epoxy, which were involved with the sulfonyl groups and the secondary hydroxyls. The intramolecular association could suppress the formation of the strong intermolecular hydrogen bonding interactions between carbonyls and hydroxyls of amine-cured epoxy, which are sufficient to fulfill the homogenization of the system during the in situ polymerization. Therefore, the presence of the intramolecular specific interactions between sulfonyl and hydroxyl groups was taken as the origin of phase-separated morphology for DDS-cured blends of epoxy with PCL.     

Miscibility of C60-end-capped poly(ethylene oxide) with poly(vinyl chloride)

The miscibility of blends of single [60]fullerene (C₆₀)-end-capped poly(ethylene oxide) (FPEO) or double C₆₀-end-capped poly(ethylene oxide) (FPEOF) with poly(vinyl chloride) (PVC) has been studied. Similar to poly(ethylene oxide) (PEO), both FPEO and FPEOF are also miscible with PVC over the entire composition range. X-ray photoelectron spectroscopy showed the development of a new low-binding-energy Cl2p doublet and a new high-binding-energy O1s peak in FPEO/PVC blends. The results show that the miscibility between FPEO and PVC arises from hydrogen bonding interaction between the α-hydrogen of PVC and the ether oxygen of FPEO. From the melting point depression of PEO, FPEO or FPEOF in the blends, the Flory-Huggins interaction parameters were found to be −0.169, −0.142, −0.093 for PVC/PEO, PVC/FPEO and PVC/FPEOF, respectively, demonstrating that all the three blend systems are miscible in the melt. However, the incorporation of C₆₀ slightly impairs the interaction between PEO and PVC.     

Miscibility of chitosan/poly(ethylene oxide) blends and effect of doping alkali and alkali earth metal ions on chitosan/PEO interaction

The miscibility of Chitosan (CS) and poly(ethylene oxide) (PEO) in their blends and the effect of K⁺ and Ca²⁺ doping on the CS/PEO interaction have been investigated in this work. CS and PEO appeared to be miscible and the DSC analysis suggested the Flory-Huggins interaction parameter χ_AB to be −0.21. Doping of K⁺ and Ca²⁺ into the CS/PEO blend matrix enhanced the cooperative interaction between CS and PEO and this enhancement was larger for Ca²⁺ than for K⁺. The difference between Ca²⁺ and K⁺ possibly reflects a stronger multi-valence interaction of Ca²⁺ with the amino and hydroxyl groups of CS as well as the ether groups of PEO to form a stable CS/Ca²⁺/PEO complex and a less significant interaction of K⁺, as suggested by DSC, WAXD and FTIR results. MD simulations clearly indicated the correlation between the dynamic behavior and the interaction of K⁺ and Ca²⁺ in the CS/PEO blend matrix.     

Intermolecular interaction in aqueous solution of binary blends of poly(acrylamide) and poly(ethylene glycol)

The interaction between poly(acrylamide) (PAM) and poly(ethylene glycol) (PEG) in their solid mixture was studied by Fourier transform infrared spectroscopy (FTIR); and their interaction in aqueous solution was investigated by nuclear magnetic resonance spectroscopy (NMR). For the solid PAM/PEG mixtures, an induced shift of the >C?O and >N? H in amide group was found by FTIR. These results could demonstrate the formation of intermolecular hydrogen bonding between the amide group of PAM and the ether group of PEG. In the aqueous PAM/PEG solution system, the PAM and PEG associating with each other in water, i.e., the amide group of PAM interacting with the ether group of PEG through hydrogen bonding was also found by ¹H NMR. Furthermore, the effects of different molecular weight of PAM on the strength of hydrogen bonding between PAM and PEG in water were investigated systemically. It was found that the hydrogen bonding interaction between PAM and PEG in water did not increase with the enlargement of the PAM molecular weight as expected. This finding together with the viscosity reduction of aqueous PAM/PEG solution with the PAM molecular weight increasing strongly indicated that PAM molecular chain, especially having high molecular weights preferred to form spherical clews in aqueous PEG solution. Therefore, fewer amide groups in PAM could interact with the ether groups in PEG. Based on these results, a mechanism sketch of the interaction between PAM and PEG in relatively concentrated aqueous solution was proposed. The fact that the phase separation of aqueous PAM/PEG solution occurs while raising the temperature indicates that this kind of hydrogen bonding between PAM and PEG in water is weak and could be broken by controlling the temperature. © 2010 Wiley Periodicals, Inc. J Appl Polym Sci, 2010     

Miscibility and morphology in crystalline/amorphous blends of poly(caprolactone)/poly(4-vinylphenol) as studied by DSC, FTIR, and C solid state NMR

The miscibility and morphology of poly(caprolactone) (PCL) and poly (4-vinylphenol) (PVPh) blends were investigated by using differential scanning calorimetry (DSC), Fourier transform infrared (FTIR) spectroscopy and ¹³C solid state nuclear magnetic resonance (NMR) spectroscopy. The DSC results indicate that PCL is miscible with PVPh. FTIR studies reveal that hydrogen bonding exists between the hydroxyl groups of PVPh and the carbonyl groups of PCL. ¹³C cross polarization (CP)/magic angle spinning (MAS)/dipolar decoupling (DD) spectra of the blends show a 1 ppm downfield shifting of ¹³C resonance of PVPh hydroxyl-substituted carbons and PCL carbonyl carbons with increasing PCL content. Both FTIR and NMR give evidence of inter-molecular hydrogen bonding within the blends. The proton spin-lattice relaxation in the laboratory frame, T₁(H), and in the rotating frame, T_1ρ(H), were studied as a function of the blend composition. The T₁(H) results are in good agreement with thermal analysis; i.e. the blends are completely homogeneous on the scale of 50-80 nm. The T_1ρ(H) results indicate that PCL in the blends has both crystalline and amorphous phases. The amorphous PCL phase is miscible with PVPh, but the PCL crystal domain size is probably larger than the spin-diffusion path length within the T_1ρ(H) time-frame, i.e. larger than 2-4 nm. The mobility differences between the crystalline and amorphous phases of PCL are clearly visible from the T_1ρ(H) data.     

Epoxy resin containing poly(ethylene oxide)-block-poly(?-caprolactone) diblock copolymer: Effect of curing agents on nanostructures

An amphiphilic diblock copolymer, poly(ethylene oxide)-block-poly(?-caprolactone) (PEO-b-PCL) was synthesized via the ring-opening polymerization of ?-caprolactone in the presence of a hydroxyl-terminated poly(ethylene oxide) monomethyl ether. The diblock copolymer was incorporated into epoxy thermosets. It is found that the formation of nanostructures of thermosetting blends is quite dependent on the uses of aromatic amine hardeners. For 4,4′-methylenebis(2-chloroaniline) (MOCA)-cured thermosetting system, the homogeneous morphology was obtained at the compositions investigated. Nonetheless, the nanostructured thermosets were obtained when the blends were cured with 4,4′-diaminodiphenylsulfone (DDS). The differential scanning calorimetry (DSC) showed that the nanostructured thermosets did not displayed any crystallinity although the subchains of the diblock copolymer are crystalline. The nanostructures were evidenced by means of atomic force microscopy (AFM), small-angle X-ray scattering (SAXS) and transmission electron microscopy (TEM). The dependence of morphological structures on the types of aromatic amines for epoxy and PEO-b-PCL thermosetting blends were interpreted on the basis of the difference in hydrogen bonding interactions resulting from the structure of curing agents. Considering the complete miscibility of the subchains (viz. PEO and PCL) with the precursors of epoxy resin before curing, it is judged that the formation of the nanostructures in the thermosets follows the mechanism of reaction-induced microphase separation, which is in marked contrast to the mechanism of self-assembly, i.e., micelle structures of block copolymers are formed prior to curing, followed by fixing these nanostructures via curing.     

Miscibility and interactions in poly(2,2,3,3,3-pentafluoropropyl methacrylate-co-4-vinylpyridine)/poly(p-vinylphenol) blends

The miscibility and specific interactions in poly(2,2,3,3,3-pentafluoropropyl methacrylate-co-4-vinylpyridine) (PFX, X=0, 28, 40 or 54, denoting the mol% of 4-vinylpyridine unit in the copolymer)/poly(p-vinylphenol) (PVPh) blends have been studied by differential scanning calorimetry (DSC), atomic force microscopy (AFM), Fourier transform infrared (FTIR) spectroscopy, and X-ray photoelectron spectroscopy (XPS). DSC studies show that PF0 is immiscible with PVPh, and the presence of a sufficient amount of 4-vinylpyridine units in the copolymer produces miscible blends. AFM images also clearly show that the blends change from heterogeneous to homogeneous upon the incorporation of 4-vinylpyridine unit into the copolymer. FTIR and XPS show the existence of inter-polymer hydrogen bonding between PFX and PVPh. The intensity of the inter-polymer hydrogen bonding increases with increasing 4-vinylpyridine content in the copolymer.     

Thermal,Spectroscopic, and Mechanical Properties of Blend Films of Poly(N-Vinyl-2-Pyrrolidone) and Sodium Alginate

Blends of poly(N-vinyl-2-pyrrolidone) (PVP) and sodium alginate (NaAlg) were prepared by casting from aqueous solutions. These blends were characterized by Fourier transform infrared spectroscopy (FT-IR), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), and tensile strength test. The miscibility in the blends of PVP and NaAlg was established on the basis of the thermal analysis results. DSC showed that the blends possessed single, composition-dependent glass transition temperatures (T _g s), indicating that the blends are miscible in amorphous state. FT-IR studies indicate that there are the intermolecular hydrogen bonding interactions, i.e., –OH·····O=C in PVP/NaAlg blends. This blend films also exhibited the higher thermal stability and improved the elongation at break in dry states.     

Hydrogen bonding effect on the poly(ethylene oxide), phenolic resin,and lithium perchlorate–based solid‐state electrolyte

The interaction behavior of solid‐state polymer electrolytes composed of poly(ethylene oxide) (PEO)/novolac‐type phenolic resin and lithium perchlorate (LiClO₄) was investigated in detail by DSC, FTIR, ac impedance, DEA, solid‐state NMR, and TGA. The hydrogen bonding between the hydroxyl group of phenolic and ether oxygen of the PEO results in higher basicity of the PEO. The higher basicity of the ether group can dissolve the lithium salts more easily and results in a greater fraction of “free” anions and thus higher ionic conductivity. DEA results demonstrated that addition of the phenolic increases the dielectric constant because of the partially negative charge on the ether group induced by the hydrogen bonding interaction between ether oxygen and the hydroxyl group. The study showed that the blend of PEO(100)/LiClO₄(25)/phenolic(15) possesses the highest ionic conductivity (1.5 × 10^?5 S cm^?1) with dimensional stability. © 2003 Wiley Periodicals, Inc. J Appl Polym Sci 91: 1207–1216, 2004     

Processable aromatic polyesters based on bisphenol derived from cashew nut shell liquid: synthesis and characterization

The miscibility of chitosan/poly(ethylene oxide) (CS/PEO) blends was investigated by a combination of experiment and molecular simulation. Results from X-ray diffraction (WAXD) and thermal analysis (DSC) suggest that the maximum miscibility was seen at the PEO weight fraction (w _PEO) =0.2; the optimum stoichiometric ratio for CS and PEO functional groups. The change in vibrational frequencies from infrared spectra was attributed to the specific interaction between PEO ether oxygen with the amino and hydroxyl groups of CS. Radial distribution functions (RDF) from MD simulation suggest that all CS functional groups (NH₂, C3-OH, and C6-OH) can interact with PEO ether groups for which NH₂ has the highest activity. For CS hydroxyl groups, a more significant contribution of C6-OH rather than C3-OH groups that interact with PEO ether oxygen was observed. The interaction parameter (χ) determined from MD simulation was in good agreement with that of the DSC experiment (χ_CS-PEO?=?-0.21). Based on a comparison between χ and χ _critical , CS/PEO blend was predicted to be miscible for w _PEO <0.58 with a maximum at w _PEO =0.2. In addition, the order parameter from the mesoscale simulation was employed to monitor the phase separation in these blends. From MesoDyn simulation, the miscibility was decreased with increasing PEO content, and miscible CS/PEO blends were obtained only with w _PEO <0.58, in good agreement with MD simulation and experiment.     

A study of blending and complexation of poly(acrylic acid)/poly(vinyl pyrrolidone)

Poly(acrylic acid) (PAA) and poly(vinyl pyrrolidone) (PVP) were chosen to prepare polymer complex and blends. The complex was prepared from ethanol solution and the blends were prepared from 1-methyl-2-pyrrolidone solution. DSC results show that the T_gs of the PAA/PVP blends lie between those of the two constituent polymers, whereas T_g of the PAA/PVP complex is higher than both blends and the two constituent polymers. TGA results show that degradation temperature, T_d, of PAA increases upon adding PVP in the blend, but thermal stability of the complex is higher than that of the blends as reflected by the higher T_d. Both FTIR and high-resolution solid state NMR show strong hydrogen bonding between PAA and PVP by showing significant chemical shift. The T_1ρ(H) measurement shows that the homogeneity scale for the blend is at ∼20 Å and that for the complex is ∼15 Å.     

Time-resolved conformational analysis of poly(ethylene oxide) during the hydrogelling process

We investigated a drastic conformation change in a poly(ethylene oxide) (PEO) chain during the hydrogelation process using infrared (IR) spectroscopy and quantum chemical calculations (QCCs). Time-resolved in situ IR spectra of the hydrogelling process of a semi-crystalline PEO solid were measured using a flow-through cell. It was found from the time-resolved IR study that gauche conformations around the C-C bonds in the crystalline phase PEO chain maintain their conformations even after hydrogelation, while at least half of the trans conformations around the C-O bonds change into gauche conformations upon hydrogelling. With regard to the phenomena of these conformation changes after contacting water, the destruction and hydrogelation of the crystalline phase around the C-C bonds of the hydrophobic moiety occur prior to changes around the C-O bonds of the hydrophilic moiety. In addition, our QCC confirmed that the stable hydration structure of bridging water, wherein the two hydroxyl groups in a water molecule donate hydrogen bonds to every other ether oxygen atoms in the PEO chain.     

Molecular modeling simulations and thermodynamic approaches to investigate compatibility/incompatibility of poly(l-lactide) and poly(vinyl alcohol) blends

This paper investigates the molecular modeling simulation approaches for understanding the blend compatibility/incompatibility of poly(l-lactide), PLL and poly(vinyl alcohol), PVA. Blends of PLL/PVA have been widely used in biotechnology as well as membranes in separation science. Realizing their importance, we thought of investigating to verify experimental observations on their compatibility/incompatibility aspects by calculating thermodynamic interactions between PLL and PVA over the entire range of blend compositions. In doing so, Flory-Huggins interaction parameter, χ, was computed for different blends using atomistic simulations to predict blend miscibility. It was found that at 1:9 blend composition of PLL/PVA, miscibility was observed, but increasing immiscibility was prevalent at higher compositions of PLL component. Computed results confirmed the literature findings on differential scanning calorimetry (DSC), Fourier transform infrared (FTIR) and mechanical property studies, suggesting the validity of modeling strategies. Plots of Hildebrand solubility parameter, δ, and cohesive energy density, CED, supported these findings. Miscibility of PLL and PVA polymers is attributed to hydrogen-bonding effect. Literature findings have been validated to understand the nature of interactions between different groups of the polymers by computing radial distribution function, RDF, for groups that are tentatively involved in such interactions, leading to miscibility or immiscibility. RDF plot was constructed to identify the exact contribution of particular atoms of polymers to confirm miscibility/immiscibility of blends. Results of this study are correlated well with the reported data. Kinetics of phase separation was examined using density profiles calculated from the MesoDyn approach to examine miscibility/immiscibility aspects of the blends. Computed free energy from the mesoscopic simulation of blends reached equilibrium, particularly when simulation was performed at higher time step, indicating the stability of the blend at certain compositions. X-ray diffraction profiles have been constructed for individual polymers as well as for their blends, which agreed well with the reported data.