Supramolecular gels can be designed such that pre-determined changes in state occur. For example, systems that go from a solution (sol) state to a gel state and then back to a sol state can be prepared using chemical processes to control the onset and duration of each change of state. Based on this, more complex systems such as gel-to-sol-to-gel and gel-to-gel-to-gel systems can be designed. Here, we show that we can provide additional insights into such systems by using rheological measurements at varying values of frequency or strain during the evolution of the systems. Since the different states are affected to different degrees by the frequency and/or strain applied, this allows us to better understand and follow the changes in state in such systems.

We use a pH-driven annealing process to convert between co-assembled and self-sorted networks in multicomponent gels. The initially formed gels at low pH are co-assembled, with the two components coexisting within the same self-assembled structures. We use an enzymatic approach to increase the pH, resulting in a gel-to-sol transition, followed by a hydrolysis to lower the pH once again. As the pH decreases, a self-sorted network is formed by a two-stage gelation process determined by the pK a of each component. This approach can be expanded to layered systems to generate many varied systems by changing composition and rates of pH change, adapting their microstructure and so allowing access to a far greater range of morphologies and complexity than can be achieved in single component systems.

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Preparation of multicomponent systems provides a method for changing the properties of low molecular weight gelator (LMWG)-based systems. Here we have prepared a variety of multicomponent systems where both components...