In order to understand the mechanisms behind the undesired a
gin
g of films based on vital wheat
gluten plasticizedwith
glycerol, films cast from water/ethanol solutions were investi
gated. The effect of pH was studied by castin
gfrom solutions at pH 4 and pH 11. The films were a
ged for 120 days at 50% relative humidity and 23
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ges/entities/de
g.
gif">C, andthe tensile properties and oxy
gen and water vapor permeabilities were measured as a function of a
gin
g time. Thechan
ges in the protein structure were determined by infrared spectroscopy and size-exclusion and reverse-phasehi
gh-performance liquid chromato
graphy, and the film structure was revealed by optical and scannin
g electronmicroscopy. The pH 11 film was mechanically more stable with time than the pH 4 film, the latter bein
g initiallyvery ductile but turnin
g brittle toward the end of the a
gin
g period. The protein solubility and infrared spectroscopymeasurements indicated that the protein structure of the pH 4 film was initially si
gnificantly less polymerized/a
ggre
gated than that of the pH 11 film. The polymerization of the pH 4 film increased durin
g stora
ge but it didnot reach the de
gree of a
ggre
gation of the pH 11 film. Reverse-phase chromato
graphy indicated that the pH 11films were to some extent deamidated and that this increased with a
gin
g. At the same time a lar
ge fraction of thea
ged pH 11 film was unaffected by reducin
g a
gents, su
ggestin
g that a time-induced isopeptide cross-linkin
g hadoccurred. This isopeptide formation did not, however, chan
ge the overall de
gree of a
ggre
gation and consequentlythe mechanical properties of the film. Durin
g a
gin
g, the pH 4 films lost more mass than the pH 11 films mainlydue to mi
gration of
glycerol but also due to some loss of volatile mass. Scannin
g electron and optical microscopyshowed that the pH 11 film was more uniform in thickness and that the film structure was more homo
geneousthan that of the pH 4 film. The oxy
gen permeability was also lower for the pH 11 film. The fact that the pH 4film experienced a lar
ger and more rapid chan
ge in its mechanical properties with time than the pH 11 film, asa consequence of a
greater loss of plasticizer, was presumably due to its initial lower de
gree of protein a
ggre
gation/polymerization. Consequently, the cross-link density achieved at pH 4 was too low to effectively retain volatilesand
glycerol within the matrix.