In this review, we focus on the types of smart supramolecular gels whose self-assembly processes are affected or even triggered by physical forces including sonication and mechanical stress (mechanical force). The types of gels that are responsive to sonication and mechanical stress are examined and summarised. The gels exhibit non-covalent interactions among the gelator molecules and show dynamic and reversible properties controlled by the stimuli. Upon stimulation, the gelators cause instant and in situ gelation of organic solvents or water with different modes and outcomes of self-assembly. On the other hand, sonication and mechanical stress, as external factors, can give rise to dynamic changes in microscopic morphology, optical properties, etc. Certain thixotropic supramolecular gels exhibit perfect self-healing characteristics. The driving forces and the mechanism of the self-assembly process and the responsive outcome of morphological and spectroscopic changes are discussed. Those supramolecular gels responding to sonication and mechanical stress offer a wide range of applications in fields such as smart and adaptive materials, switches, drug control and release, and tissue engineering.
Two new peptide-based isomers containing cholesterol and naphthalic groups have been designed and synthesized. We found that the position of L-alanine in the linker could tune the gelation properties and morphologies. The molecule with the L-alanine residue positioned in the middle of the linker (1b) shows better gelation behavior than that with L-alanine directly linked to the naphthalimido moiety (1a). As a result, a highly thermostable organogel of 1b with a unique core-shell structure was obtained at high temperature and pressure in acetonitrile. Moreover, the gels of 1a and 1b could undergo an instantaneous gel-to-gel transition triggered by sonication. Ultrasound could break the core-shell microsphere of 1b and the micelle structure of 1a into entangled fibers. By studying the mechanism of the sonication-triggered gel-to-gel transition process of these compounds, it can be concluded that ultrasound has a variety of effects on the morphology, such as cutting, knitting, unfolding, homogenizing, and even cross-linking. Typically, ultrasound can cleave and homogenize pi-stacking and hydrophobic interactions among the gel molecules and then reshape the morphologies to form a new gel. This mechanism of morphology transformation triggered by sonication might be attractive in the field of material storage and controlled release.
A naphthalimide-based fluorescent gelator (N1) containing an alkenyl group has been designed and characterized. This material is able to gelate alcohols via a precipitate-to-gel transformation when triggered with ultrasound for less than 2 min (S-gel). The gelation process in n-propanol was studied by means of absorption, fluorescence, and IR spectra, scanning electron microscopy (SEM) images, and X-ray diffraction patterns. The fluorescence intensity of N1 decreased during the gelation process in a linear relationship with the sonication time. The S-gel of N1 could be used to sense aliphatic and aromatic amines by measuring the change in the signal output. For example, the addition of propylamine to the S-gel of N1 resulted in a dramatic enhancement of the fluorescence intensity, accompanied by a gel-to-sol transition. On the contrary, when the S-gel of N1 was treated with aromatic amines such as aniline, fluorescence was quenched and there was no gel collapse. The sensing mechanisms were studied by (1)H NMR, small-angle X-ray scattering, SEM and spectroscopic experiments. It is proposed that isomerization of the alkenyl group of N1 from the trans to cis form occurs when the S-gel is treated with propylamine, resulting in a gel-sol transition. However, the aromatic aniline molecules prefer to insert into the gel networks of N1 via hydrogen-bonding and charge-transfer interactions, maintaining the gel state. As potential applications, testing strips of N1 were prepared to detect aniline.
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