Spatially resolved polymer mobilization revisited - Three-dimensional, UltraShort Echo Time (3D UTE) magnetic resonance imaging of sodium alginate matrix tablets

J Colloid Interface Sci. 2023 Nov:649:626-634. doi: 10.1016/j.jcis.2023.06.139. Epub 2023 Jun 20.

Abstract

Hypothesis: Three-dimensional 1H UltraShort Echo Time magnetic resonance imaging (1H 3D UTE MRI) of the matrix tablet made of hydrophilic polymer hydrated in heavy water (D2O) will allow investigation of the hydration-induced spatiotemporal evolution of the material originally included in the matrix tablet during manufacturing (i.e., polymer chains and bound water).

Experiments: The oblong-shaped sodium alginate matrix tablets were used to verify the hypothesis. The matrix was measured before and during hydration in D2O for up to 2 h using the 1H 3D UTE MRI. Five echo times (first at 20 μs) were used, resulting in five three-dimensional images (one image for each echo time). In chosen cross-sections, two parametric images, i.e., amplitude and T2* relaxation time maps, were calculated using "pixel-by-pixel" mono-exponential fitting.

Findings: The regions of the alginate matrix with T2* shorter than 600 μs were analyzed before (air-dry matrix) and during hydration (parametric, spatiotemporal analysis). During the study, only hydrogen nuclei (protons) pre-existing in the air-dry sample (polymer and bound water) were monitored because the hydration medium (D2O) was not visible. As a result, it was found that morphological changes in regions having T2* shorter than 300 μs were the effect of fast initial water ingress into the core of the matrix and subsequent polymer mobilization (early hydration providing additional 5% w/w hydration medium content relating to air-dry matrix). In particular, evolving layers in T2* maps were detected, and a fracture network was formed shortly after the matrix immersion in D2O. The current study presented a coherent picture of polymer mobilization accompanied by local polymer density decrease. We concluded, that the T2* mapping using 3D UTE MRI can effectively be applied as a polymer mobilization marker.

Keywords: Alginates; Hydrophilic polymers; Magnetic resonance imaging (MRI); Mass transport; Polymer hydration; Polymer relaxation; Short T(2) relaxation times; Swelling, polymer mobilization; Ultrashort Echo Time (UTE).