The study of composition-properties relationships for composite hydrogels based on poly(methacrylic acid) and high concentrations of MFI zeolite

High concentrations of hydrophobic MFI zeolite (26.0–51.3 wt%) were successfully embedded in poly(methacrylic acid) (PMAA) network in simple, one-pot synthesis of PMAA-MFI composite hydrogels. The effects of zeolite concentration regarding pure PMAA xerogel, for all of the investigated properties (primary structural parameters, morphological properties, water swelling ability, thermal degradation mechanism and stability, and mechanical properties) were determined and discussed. The PMAA-MFI composite hydrogels had remarkably higher density than PMAA xerogel (1660/1420 kg m−3), higher crosslinking density (29/1.0 × 10−4), improved mechanics in the dry and swollen state (up to 4.9 times higher storage modulus) and lower swelling degree (42/420 g g−1), average molar mass between the network crosslinks (3.6/110 × 104 g mol−1), and distance between the macromolecular chains (64/710 nm). Despite high zeolite concentration, the composites kept porous hydrogel structure with uniformly dispersed zeolite particles. FTIR spectra disclosed the existence of functional groups of PMAA network and MFI zeolite that interacted mutually and led to increased crosslinking density. The effect of zeolite concentration on the thermal degradation mechanism was established. The composition-properties correlations were determined and described by the adequate linear or power law equations revealing the additive nature of the composites and the fractal structure of the networks. These correlations enable the achievement of desired properties by simple adjustment of the initial composition, i.e. zeolite concentration. Therefore, this work presents the base for further development of tailor-made PMAA-MFI composite hydrogels aimed for specific application.