This work explores confocal Raman microscopy as a novel approach to study the microstructure of oleogels, using milk fat-based oleogels as a case study. Anhydrous milk fat (AMF) was sequentially fractionated to obtain two olein and two stearin fractions with different thermal properties. These and the unfractionated AMF were structured into oleogels using ethyl cellulose as gelling agent. Although the fatty acid profile of the different fractions showed only minor changes (in most cases < 10% change), the microstructure of the various oleogels was markedly different, especially the unfractionated AMF based oleogels, which exhibited distinct pseudo-spherical features suggesting segregation of components. Different univariate and multivariate data analysis approaches, were compared to map the distribution of components in the oleogels using confocal Raman microscopy. The univariate approach only provided accurate microstructural information for oleogels prepared with olein (liquid at the temperature of analysis). The multivariate approaches, although more complex, provided reliable...

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