Luminescent lanthanide-containing gelatin/polydextran/laponite nanocomposite double-network hydrogels for processing and sensing applications

Lanthanide-containing nanomaterials have gained significant popularity for their utilization in polymeric networks, enabling the creation of luminescent nanocomposites for advanced applications. In this study, we developed a new type of lanthanide-containing nanocomposite hydrogels by incorporating terbium-containing laponite (Tb3+@Lap) into the networks of polyethyleneimine-modified gelatin/polydextran aldehyde (PG/ PDA) through dynamic bonds. The structures and properties of the Tb3+@Lap-containing nanocomposite doublenetwork (ncDN) hydrogels were comprehensively investigated in comparison with the DN hydrogels with a pure polymeric network and the Lap-containing ncDN hydrogels. The PG/PDA/Tb3+@Lap ncDN hydrogels with multiple dynamic bonds (i.e., imine bonds, coordination bonds, hydrogen bonds, and electrostatic interactions) exhibited remarkable characteristics of shear-thinning and self-healing, making them suitable for the construction of hydrogel scaffolds on a macroscale using fabrication techniques such as electrospinning and 3D printing. Moreover, the PG/PDA/Tb3+@Lap ncDN hydrogels have been demonstrated to act as sensitive and selective luminescent sensors for detecting copper ions. Taken together, a versatile lanthanide-containing ncDN hydrogel platform capable of dynamic features is developed for processing and sensing applications.