Switchable Supramolecular Configurations of Al3+/LysTPY Coordination Polymers in a Hydrogel Network Controlled by Ultrasound and Heat

Coordination-driven self-assembly with controllable properties has attracted increasing interest because of its potential in biological events and material science. Herein, we report on the remote, instant, and switchable control of competitive coordination interactions via ultrasound and heat stimuli in a hydrogel network. Configurational coordination changes result in the transformation of blue-emissive and opaque Al³⁺-amide aggregations to yellow-green-emissive and transparent Al³⁺-terpyridine aggregations. Interestingly, circularly polarized luminescence "off-on" switches of the metallo-supramolecular assembly are also created by these configuration changes. Additionally, the impact of the stoichiometric ratio of Al³⁺ and LysTPY on the assembly is also studied in detail. With a higher content of Al³⁺, the hydrogel with branched and abundant junctions exhibited robust, self-healing, and self-supporting properties. This in-depth understanding of the coordination interaction adjustment will afford new insights into the preparation of stimuli-responsive metallogels.