A novel strategy to construct hydrogels with anti-swelling and water-retention abilities by covalent surface modification.

Hydrogels have been widely used in various fields due to their diverse properties and flexible preparation methods. However, limited by the open network structure, hydrogels inevitably lose water in air or absorb water in aqueous solution, resulting in the loss of intrinsic functions, which severely hinders their practical applications. To address this issue, a general strategy was developed by subsequently modifying the surface of hydrogels with branched polyethyleneimine (PEI) and (3-(methacryloxy)propyl)trimethoxysilane (MPS) to covalently construct a dense cross-linked siloxane layer on the hydrogel surface. As a proof of concept, poly(2-(dimethylamino)ethyl methacrylate)/sodium alginate (PDMAEMA/SA) hydrogels were chosen as the model hydrogels to verify the feasibility of this strategy. The hydrogels adsorbed PEI to form amino-rich surfaces through hydrogen bonding, followed by covalently grafting MPS through rapid and catalyst-free mutual chemical reactions between acrylates and amine groups, as well as the hydrolysis of MPS. After modification, robust hydrophobic surfaces were successfully fabricated on the hydrophilic hydrogels. The modified hydrogels exhibited extraordinary anti-swelling and water-retention abilities. As the most typical intrinsic properties of hydrogels, the conductivity and sensing performance were well preserved. The strategy reported here provides a new insight into the construction of hydrogels with anti-swelling and water-retention abilities.