Open porous polymeric materials have gained popularity due to their exceptional properties and applications in tissue engineering scaffolds, drug delivery, enzyme immobilization and catalysis support. This study developed a novel two-stage approach to create networked, crosslinked poly(2-hydroxyethyl methacrylate-co-N,N'-methylenebisacrylamide) HEMA-MBA beads. The first part involves producing an oil-in-water-in-oil high internal phase emulsion (HIPE). This is followed by suspension polymerization using a redox initiator pair. In this study, a mixed surfactant combination with low and high hydrophilicity-lipophilicity balance surfactants was identified and successfully utilized to prepare a stable oil-in-water-in-oil HIPE. The effect of crosslinker concentration (i.e. crosslink density), surfactant concentration and monomer-to-porogen ratio on pore architecture and surface area were successfully evaluated. In addition, a new protocol was developed to synthesize HEMA-MBA monoliths using an oil-in-water HIPE method at ambient temperature using a redox initiator pair. The effect of crosslink density and oil phase on pore architecture and surface area was evaluated. Key variables affecting the morphology of porous HEMA-MBA beads and monoliths were identified and quantified, allowing future development of porous HEMA-based polymer beads and monoliths with tunable morphologies which are suitable for numerous applications, especially in the biomedical field. (c) 2022 Society of Industrial Chemistry.

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