Effect of expanded graphite on the thermal conductivity of sodium sulfate decahydrate (Na2SO4·10H2O) phase change composites

Inorganic salt hydrate phase change materials (PCMs) are of interest for near-room temperature thermal energy storage (TES) systems, but their low thermal conductivity, ~ 0.5 W/m-K, limits their performance. In this work, we report the thermal conductivity and bulk density of composites containing sodium sulfate decahydrate (SSD) Na2SO4·10H2O with three types of graphite: expanded graphite (EG), milled EG (MG), and graphite nanoplatelets (GnP). The effect of these thermophysical properties on TES performance is presented. The composites were made using a readily scalable one-pot synthesis procedure with graphite received as-is. A 583% increase in thermal conductivity (4.1 W/m-K) was achieved with 25 wt% EG. However, as EG fraction increases, bulk density decreases and thermal conductivity plateaus. This ultimately resulted in lower thermal performance at higher EG fractions despite higher thermal conductivity. This highlights the tradeoff between PCM composite properties and performance, and why thermal conductivity is insufficient to describe PCM thermal performance. GnP is added to EG-SSD to increase bulk density and energy storage density, but these density improvements do not offset lower thermal conductivity and thus thermal performance declined. Similarly, MG-SSD composites had a higher bulk density and energy storage density, but lower thermal conductivity and thermal performance than EG-SSD composites at similar compositions. Atomistic molecular dynamics simulations were performed to understand the structure-property relationship of graphite-SSD interfaces. The simulations support the hypothesis that atomic level contact resistance between graphite and SSD increases thermal resistance at the interfaces resulting in effectively lower bulk thermal conductivity in MG-SSD compared to EG-SSD.