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Molecules 2020, 25, 5572 8 of 26 Figure 7. (A) Peak melting points ( ◦C) collected in literature of the α (black, round), β’ (red, diamond) and β (blue, triangle) phases of saturated symmetrical triglycerides plotted against the carbon number of the precursor fatty acids (between 8 and 24). A clear alternation between odd- and even-numbered triglycerides can be observed for the β phases, while it is absent in the α and barely noticeable in the β’ phase. (B) Difference between the average melting points of the polymorphic phases plotted against the carbon number of the precursor fatty acids (between 8 and 24). A clear reduction in the differences between the melting points of each phase can be seen for increasing carbon numbers, indicating that the polymorphs have more similar behaviour to each other for longer triglycerides. Another trend observed for SST is the alternation in the melting points of the β- and β’-phases of triglycerides derived from odd-numbered or even-numbered fatty acids (Figure 7A). This behaviour has previously been reported by Malkin [24] and Lutton [15] and is also reflected in the variation between the melting points of the crystalline phases shown in in Figure 7B. Boese et al. [42,43] and Ravotti et al. [44] have also reported this for alkanes and saturated fatty esters. The reason behind such alternation in the melting points is attributed to odd-numbered carbon chains’ lower degree of symmetry and less optimal intermolecular interactions compared to even-numbered chains. However, this effect is only clearly visible for the β-phase, whereas for the β’-phase it is negligible, and it is completely absent in the α-phase, where melting points are only seen increasing with increasing carbon numbers. Malkin [24] attributed this behaviour to a change in the long d-spacings in tilted odd-numbered molecules (Figure 8). As can be seen, due to a lack of tilting of the molecules in the α-phase, the long spacings result affected only in the β’ and β phase. In particular, a greater tilt of approximately 65◦ occurs in the β phase. Compared to the melting points, very limited data are available concerning the enthalpies of fusion of SST. Several studies have focused on the temperatures at which the phase change occurs, however they do not mention the phase change enthalpy. Furthermore, there is considerable variation in the reported values, reflecting the lack of precision and variability of experimental measurements. It is generally unclear how the enthalpies of fusion are obtained when polymorphism is apparent, and in some cases there is no mention of which polymorph is being studied [29]. This clearly emphasizes the need for additional, systematic investigations on this class of materials. Nevertheless, some trends can be observed for these SSTs. In general, the enthalpy of fusion (∆H) increases with increasing numbers of carbon atoms and differs significantly between different polymorphs (Figure 9).PDF Image | Triglycerides as Novel Phase-Change Materials
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