Interfacial layer properties and enthalpy relaxation of polymer nanocomposites: Effect of nanoparticle dispersion

Abstract Investigating the effect of nanoparticle dispersion morphology on the properties of the interfacial layer of polymer nanocomposites (PNCs) provides an important theoretical basis for designing and regulating the macroscopic properties of PNCs. Differential scanning calorimetry (DSC) and broadband dielectric spectroscopy (BDS) were used to investigate the characteristic parameters of the interfacial area, segmental dynamics and enthalpy relaxation of PNCs with nanoparticle agglomerates and uniformly dispersed morphology. The volume fraction of the interfacial area ( φ _int ) and the extent of influence of the interfacial area on the enthalpy hysteresis reduction ( χ _int ) in PNCs with agglomerated nanoparticles are lower than that of PNCs with uniformly dispersed nanoparticles for the same nanoparticle loading. Because of the irregular structure of the nanoparticle aggregate morphology, the linear relationships between φ _int and nanoparticle content is not valid in PNCs with agglomerated nanoparticles. Interestingly, φ _int obtained by BDS and χ _int have a clearly linear relationship in all PNCs, independent of nanoparticle dispersion morphology. Such universal quantitative relationship provides a new research methodology for investigating the characteristic parameters of the interfacial area in PNCs, and facilitates the construction of a correspondence between the microscopic parameters of interfacial area and the macroscopic properties of PNCs. Highlights The linear relationships between φ _int and nanoparticle content are not valid in PNCs with agglomerated nanoparticles. The linear relationships between φ _int and the decreased degree of Δ H _R can be noted in all PNCs, independent of nanoparticle dispersion morphology. The universal correspondence provides a new research methodology for investigating the characteristic parameters of the interface layer in PNCs.