Aging and metastability of monoglycerides in hydrophobic solutions

TL;DR

This study investigates how monoglycerides in hydrophobic solutions age and lose their emulsifying ability over time due to changes in hydrogen bonding and molecular arrangement, leading to structural reordering and collapse of gel networks.

Contribution

It provides a comprehensive analysis of the aging process of monoglycerides in hydrophobic media using multiple techniques, revealing the molecular mechanisms behind structural changes.

Findings

Monoglycerides lose emulsifying ability as hydrogen bonding patterns change.

Aging causes segregation of D and L isomers within bilayers.

Structures eventually reorder into beta-crystalline state, weakening gel networks.

Abstract

The aging of aggregated structures of monoglycerides in hydrophobic medium is described by a set of different techniques. Polarized microscopy was used to study the mesomorphic behavior as a function of time. Differential scanning calorimetry was utilized to quantitatively monitor changes in the latent heat in different phase transformations that take place in the aging system. Infrared spectroscopy was applied to detect the formation of hydrogen bonding between surfactants. The X-ray diffraction patterns fingerprinted the molecular arrangement in different emerging phases. Infra-red spectroscopy was used to monitor the state of hydrogen bonding in the system. We conclude that in both inverted-lamellar and sub-alpha crystalline phases, monoglyceride molecules inevitably lose their emulsified ability in the hydrophobic solutions through the gradual change in hydrogen bonding patterns. On aging, the formation of intermolecular hydrogen bonding between glycerol groups causes the segregation of chiral (D and L) isomers within the bilayers. Therefore all structures were eventually forced to reorder into the beta-crystalline state, distinguishing between the D and L layers. Accordingly, the highly ordered packing of aged structures weakened the emulsifying ability and finally leaded the collapse of the percolating gel network.