It is crucial for hydrogel preparation to find appropriate gelators. Fatty acids are widely distributed in nature, and thus their utilization has received much attention. In this study, we demonstrated that poly (α,L-lysine) with polymerization degree as 5 (PLL 5 ) can bind to sodium salts of fatty acids (SFA) with intermediate sizes such as sodium laurate (SL) through non-covalent interactions. Such binding resulted in SL polymerization. TEM analyses revealed that long, thin fibers initially formed upon mixing PLL 5 with SL, becoming thick and entangled after 12 h, and finally leading to the formation of limpid hydrogels. In contrast, other SFA could not form such hydrogel under the same experimental conditions. Except for PLL 5 , PLL 7 also induced SL self-assembly into similarly limpid hydrogels, while its other analogues with smaller or larger size did not. Thus, the formation of this limpid hydrogel presented here exhibited high selectivity for the size of both SFA and poly (α,L-lysine).These findings might be beneficial for application of fatty acids in industry.
IntroductionHydrogels are super-water-absorbent natural or synthetic polymer systems, which can pass the "inversion test"-turn a vial of hydrogel upside down and it is able to support its own weight without falling down. 1 Though there are several other definitions, hydrogels are essentially two-component mixtures of a small amount (typically less than 2% by weight) usually of a polymer gelator forming a network immobilizing a much larger mass of water by surface tension or capillary force. 2 The three-dimensional networks of hydrogels are usually formed by cross-linking polymer chains through covalent bonds, hydrogen bonding, van der Waals interactions, or physical entanglements. 3, 4 By imitating protein and self-assembly materials studies, 5,6 Estroff and Hamilton 2 broke down a hydrogel into a primary, secondary, and tertiary structure for better understanding of its formation mechanism. The primary structure of the hydrogel is determined by the molecular level recognition events that promote anisotropic aggregation in one or two dimensions of gelator molecules. And the morphology of the aggregates is the secondary structure, namely, micelles, vesicles, fibers, ribbons, or sheets, which is directly influenced by the primary structure. The tertiary structure of the hydrogel is defined as the interaction of individual aggregates, which determines whether a hydrogel can be formed.Networks immobilizing mass of water endows hydrogels with the ability to protect drugs or functional factors from hostile environments and to release them in response to environmental stimuli such as change of temperature or pH. Because of these interesting properties, hydrogels have been studied extensively over the past 9 entropy. This result is opposite to a recent report where sodium dodecyl sulfate (SDS) was found to bind to PLL 5 with a negative ∆S° and a negative ∆H°, 22 and thus the reaction appears to be driven by enthalpy. Both SDS and SL molecules have a long h...