Nanosilica Gel-Stabilized Phase-Change Materials Based on Epoxy Resin and Wood’s Metal

The emulsification of a molten fusible metal alloy in a liquid epoxy matrix with its subsequent curing is a novel way to create a highly concentrated phase-change material. However, numerous challenges have arisen. The high interfacial tension between the molten metal and epoxy resin and the difference in their viscosities hinder the stretching and breaking of metal droplets during stirring. Further, the high density of metal droplets and lack of suitable surfactants lead to their rapid coalescence and sedimentation in the non-cross-linked resin. Finally, the high differences in the thermal expansion coefficients of the metal alloy and cross-linked epoxy polymer may cause cracking of the resulting phase-change material. This work overcomes the above problems by using nanosilica-induced physical gelation to thicken the epoxy medium containing Wood’s metal, stabilize their interfacial boundary, and immobilize the molten metal droplets through the creation of a gel-like network with a yield stress. In turn, the yield stress and the subsequent low-temperature curing with diethylenetriamine prevent delamination and cracking, while the transformation of the epoxy resin as a physical gel into a cross-linked polymer gel ensures form stability. The stabilization mechanism is shown to combine Pickering-like interfacial anchoring of hydrophilic silica at the metal/epoxy boundary with bulk gelation of the epoxy phase, enabling high metal loadings. As a result, epoxy shape-stable phase-change materials containing up to 80 wt% of Wood’s metal were produced. Wood’s metal forms fine dispersed droplets in epoxy medium with an average size of 2–5 µm, which can store thermal energy with an efficiency of up to 120.8 J/cm³. Wood’s metal plasticizes the epoxy matrix and decreases its glass transition temperature because of interactions with the epoxy resin and its hardener. However, the reinforcing effect of the metal particles compensates for this adverse effect, increasing Young’s modulus of the cured phase-change system up to 825 MPa. These form-stable, high-energy-density composites are promising for thermal energy storage in building envelopes, radiation-protective shielding, or industrial heat management systems where leakage-free operation and mechanical integrity are critical.