Syntactic foams (SFs) combining an epoxy resin and hollow glass microspheres (HGM) feature a unique combination of low density, high mechanical properties, and low thermal conductivity which can be tuned according to specific applications. In this work, the versatility of epoxy/HGM SFs was further expanded by adding a microencapsulated phase change material (PCM) providing thermal energy storage (TES) ability at a phase change temperature of 43 °C. At this aim, fifteen epoxy (HGM/PCM) compositions with a total filler content (HGM + PCM) of up to 40 vol% were prepared and characterized. The experimental results were fitted with statistical models, which resulted in ternary diagrams that visually represented the properties of the ternary systems and simplified trend identification. Dynamic rheological tests showed that the PCM increased the viscosity of the epoxy resin more than HGM due to the smaller average size (20 µm vs. 60 µm) and that the systems containing both HGM and PCM showed lower viscosity than those containing only one filler type, due to the higher packing efficiency of bimodal filler distributions. HGM strongly reduced the gravimetric density and the thermal insulation properties. In fact, the sample with 40 vol% of HGM showed a density of 0.735 g/cm3 (−35% than neat epoxy) and a thermal conductivity of 0.12 W/(m∙K) (−40% than neat epoxy). Moreover, the increase in the PCM content increased the specific phase change enthalpy, which was up to 68 J/g for the sample with 40 vol% of PCM, with a consequent improvement in the thermal management ability that was also evidenced by temperature profiling tests in transient heating and cooling regimes. Finally, dynamical mechanical thermal analysis (DMTA) showed that both fillers decreased the storage modulus but generally increased the storage modulus normalized by density (E′/ρ) up to 2440 MPa/(g/cm3) at 25 °C with 40 vol% of HGM (+48% than neat epoxy). These results confirmed that the main asset of these ternary multifunctional syntactic foams is their versatility, as the composition can be tuned to reach the property set that best matches the application requirements in terms of TES ability, thermal insulation, and low density.
Epoxy/hollow glass microsphere (HGM) syntactic foams (SFs) are peculiar materials developed to combine low density, low thermal conductivity, and elevated mechanical properties. In this work, multifunctional SFs endowed with both structural and thermal management properties were produced for the first time, by combining an epoxy matrix with HGM and a microencapsulated phase change material (PCM) having a melting temperature of 43 °C. Systems with a total filler content (HGM + PCM) up to 40 vol% were prepared and characterized from the mechanical point of view with a broad experimental campaign comprising quasi-static, impact, and fracture toughness tests. The experimental results were statistically treated and fitted with a linear model, to produce ternary phase diagrams to provide a comprehensive interpretation of the mechanical behaviour of the prepared foams. In quasi-static tests, HGM introduction helps to retain the specific tensile elastic modulus and to increase the specific compressive modulus. The brittle nature of HGMs decreases the Charpy impact properties of the SFs, while the PCM insertion improve their toughness. This result is confirmed in KIC and GIC tests, where the composition with 20 vol% of PCM shows an increase of 80% and 370% in KIC and GIC in to neat epoxy, respectively. The most promising compositions are those combining PCM and HGMs with a total particle volume fraction up to 40 vol%, thanks to their optimal combination of thermal management capability, lightness, thermal insulation, and mechanical properties. The ability to fine-tune the properties of the SFs, together with the acquired thermal energy storage (TES) capability, confirm the great potential of these multifunctional materials in automotive, electronics, and aerospace industries.
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