This paper describes the preparation of new PEG6000-silica-MWCNTs composites as shape-stabilized phase change materials (ssPCMs) for application in latent heat storage. An innovative method was employed to obtain the new organic-inorganic hybrid materials, in which both a part of the PEG chains, used as the phase change material, and a part of the hydroxyl functionalized multiwall carbon nanotubes (MWCNTs-OH), used as thermo-conductive fillers, were covalently connected by newly formed urethane bonds to the in-situ-generated silica matrix. The study's main aim was to investigate the optimal amount of PEG6000 that can be added to the fixed sol-gel reaction mixture so that no leakage of PEG occurs after repeated heating-cooling cycles. The findings show that the optimum PEG6000/NCOTEOS molar ratio was 2/1 (~91.5% PEG6000), because both the connected and free PEG chains interacted strongly with the in-situ-generated silica matrix to form a shape-stabilized material while preserving high phase-transition enthalpies (~153 J/G). Morphological and structural findings obtained by SEM, X-ray and Raman techniques indicated a distribution of the silica component in the amorphous phase (~27% for the optimum composition) located among the crystalline lamellae built by the folded chains of the PEG component. This composite maintained good chemical stability after a 450-cycle thermal test and had a good storage efficiency (~84%).
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