Acrylamide monomers in universal adhesives

Abstract

Objectives: The mono-functional monomer 2-hydroxyethyl methacrylate (HEMA) is often added to universal adhesives (UAs) to improve surface wetting and prevent phase separation. Nevertheless, HEMA promotes water sorption and hydrolysis at adhesive interfaces, hereby affecting long-term bonding to dentin. This study investigated if two acrylamide monomers could replace HEMA in an UA formulation applied in etch-and-rinse (2E&R) and self-etch (1SE) bonding mode.

Methods: Four experimental UAs were bonded to bur-cut dentin. In addition to 12 wt% 10-MDP, 25 wt% Bis-GMA and 10 wt% TEGDMA as common monomer composition, 20 %wt ethanol and 15 %wt water as solvent, and 3 wt% polymerization-related additives, the four formulations solely differed for either the acrylamide cross-linker monomer 'FAM-201' as TEGDMA alternative and HEMA replacement, the hydroxyethyl acrylamide monomer 'HEAA' as HEMA alternative, HEMA ('HEMA+'), or extra TEGDMA in a HEMA-free control ('HEMA-'), all added in a 15 wt% concentration. The split-tooth study design involved application in 2E&R mode on one tooth half versus 1SE mode on the corresponding half. Micro-tensile bond strength of half of the micro-specimens was measured upon 1-week distilled water storage ('immediate' 1w μTBS), with the other half measured after additional 6-month storage ('aged' 6 m μTBS). Statistics involved linear mixed-effects (LME) modelling (p < .05). Additionally, interfacial TEM characterization, thin-film (TF) XRD surface analysis, LogP determination, and a cytotoxicity assay were carried out.

Results: FAM-201 revealed significantly higher μTBS than HEMA+ at 1w and 6 m when applied both in E&R and SE bonding modes. HEAA's μTBS was significantly lower than that of HEMA+ at 1w when applied in SE mode. TF-XRD and TEM revealed similar chemical and ultrastructural interfacial characterization, including stable 10-MDP_Ca salt nano-layering. FAM-201 was least cytotoxic and presented with an intermediary LogP, while HEAA presented with the highest LogP, indicating high hydrophilicity and water-sorption sensitivity.

Significance: The acrylamide co-monomer FAM-201 could replace HEMA in an UA formulation, while HEAA not.

Keywords: Acrylamides; Bond strength; Durability; HEMA; Linear mixed-effects model (LME); TEM.