Sorption heat storage technology has recently sparked an increasing interest because of its advanced heat storage capabilities. However, material-level heat and mass transfer challenges persist. This work contributes to the field by the development of new sorption composite materials that are comprised ionic liquids (1-ethyl-3-methylimidazolium methanesulfonate and 1-ethyl-3-methylimidazolium chloride) impregnated in 1–5 2D-layered graphene host matrix. Their sorption, heat transfer, heat storage, and charging/discharging rate properties were experimentally investigated using both water and ethanol as adsorbates. The adsorption isotherms and kinetics for both the adsorbates onto the developed composites and the parent ionic liquids were experimentally measured at different temperatures. The isosteric heat of adsorption for all the studied pairs was determined using the Clausius-Clapeyron method, showing an increasing trend with an increasing uptake. They showed that the specific heat storage capacity reached 187.5 kJ/kg when water was used as the working sorption agent. The corresponding heat charging/discharging rates are significantly higher, 69 %-78 %, than pure ionic liquids. Compared to silica gel as a baseline sorbent, ionic liquid-graphene composites’ heat storage and transfer capacities are higher by three orders of magnitude. The thermal diffusivities of the developed composites were significantly higher than the baseline silica gel. These innovative sorption composites show great potential for improving thermal energy storage efficiency, making them suitable for applications in renewable energy systems, industrial processes, waste heat recovery, and climate control solutions. However, the developed composites achieved inferior performance compared to the silica gel baseline sorbent when using ethanol as a working fluid to utilise sub-zero ambient air as a heat source because of the relatively larger molecular size of ethanol.
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