Temperature-Dependent Growth of Gelatin−Poly(galacturonic acid) Multilayer Films and Their Responsiveness to Temperature, pH, and NaCl

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Abstract

Temperature-dependent formation of gelatin−poly(galacturonic acid) (PGA) multilayer films based on the layer-by-layer approach and their stability to changes in temperature, pH, and NaCl concentration were investigated for the first time using quartz crystal microbalance with dissipation monitoring (QCMD). Changes in the viscoelastic properties of the gelatin−PGA films with temperature were also observed using atomic force microscopy (AFM). Four different assembly temperatures ranging from 20 to 37 °C were chosen, and the findings revealed that the assembly temperature was crucial to gelatin−PGA multilayer film formation. The highest amount adsorbed and consequently the thickest gelatin−PGA assemblies were formed at 20 °C, whereas limited growth was observed for gelatin−PGA films assembled at 37 °C. Although the experimental conditions favored electrostatic interactions to be the driving force during the gelatin−PGA assembly, the inhibited multilayer growth observed for layers formed at the temperature of 30 and 37 °C clearly indicated very weak electrostatic interactions between gelatin and PGA and the continuous multilayer growth at lower temperatures was mainly due to hydrogen bonding. The stability of assembled gelatin−PGA multilayer films to various environmental stresses was found to be significantly influenced by the changes in temperature. At low temperatures the behavior of gelatin was dominated by helix formation and association through hydrogen bonding. Raising the temperature promoted melting of the helix, disruption of the multilayer network, and disassembly of the films, which was also indicated by AFM study. In terms of the responsiveness to pH and salt, this study showed that gelatin−PGA multilayer films fabricated at 20 °C underwent almost completely reversible alternate (de)swelling changes. In contrast, gelatin−PGA multilayer films formed at 25 °C showed a partial decomposition when exposed to various pH and salt concentrations.

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