Model systems composed of tristearin in solid state and tricaprin in liquid state with different solid-fat content (SFC) and storage time have been investigated by relaxation NMR and NMR diffusometry. The T(2) relaxation of the tricaprin in the melt exhibited a bimodal distribution as previously observed. The SFC had a major effect on the T(2) relaxation. This effect was explained according to the fast diffusive exchange model in porous media. According to this model the changes in T(2) relaxation as a function of the SFC and storage time were explained by the decrease of the surface-to-volume ratio of the crystal induced by Ostwald ripening. The diffusion coefficient D of the tricaprin in the melt decreased for higher SFC. Since no significant variation of D was observed for different diffusion time, D reflected the long-range connectivity and the tortuosity was calculated. During storage the diffusion coefficient remained constant.

It is very important to monitor the characteristics of triacylglycerol crystal network in fats, as these crystals have an impact on many food properties such as texture, sensory taste, and extended shelf life. Although time-domain NMR (TD-NMR) is now the reference technique to determine the solid fat index in food, the entire possibilities of this technique are not used. Some NMR studies have been performed to determine its power for the discrimination of polymorphism. In this study, extended investigations proved that TD-NMR could evaluate triacylglycerol (TA) polymorphism, independently from temperature and chain length. Study of the dipolar interactions through second moment M(2), which is characteristic of proton mobility in solid-state samples, provided a new understanding of the structural organization of crystal molecules. Proton spin-lattice relaxation, which has been proved to be a true probe of polymorphism, has provided information on crystal networks. Combination of the two techniques revealed two very interesting kinds of results, i.e. the presence of a minimum spin-lattice relaxation time T(1) for tristearin alpha, which is a characteristic of a dynamic molecular process, and differences in behavior between long and short chain lengths, both at a molecular and a crystal level.

Fat crystal networks confer their physical properties on fat-containing products. They are characterized by the solid fat content (SFC) and the design of the crystals, that is, their polymorphism and their size. Different techniques such as NMR, differential scanning calorimetry, and X-ray diffraction (XRD) are used to determine these parameters. Low-field NMR, the reference method for evaluation of SFC, has been proven to allow the determination of polymorphism through spin-lattice relaxation time (T 1 ) and second moment (M 2 ) measurements. However, this technique could provide more information on the system. On the basis of the effects of supercooling on the NMR parameters, the first evidence of a possible relationship between the size of the crystals and T 1 was demonstrated. The effects of a liquid phase on the fat crystal network were investigated with liquid tricaprin and solid tristearin. It was demonstrated that the two triacylglycerols can cocrystallize, and that the liquid phase modified the polymorphic behavior of tristearin. The evolution of T 1 over time could be related to the Ostwald ripening phenomenon. In view of this evidence, it was concluded that there was a relationship between T 1 and the size of the crystals in the fat crystal network.