Interfacial and Mechanical Behavior of Functionalized Short Quartz Fibers via Thiol-Ene Click Chemistry for Dental Resin Composites: A Combination of Simulation and Experiment

Abstract

The development of dental resin composites (DRCs) with high mechanical performance remains a significant challenge due to the weak filler-matrix interfacial bonding. Herein, we proposed a rational strategy for interfacial reinforcement by grafting methacrylate-polyhedral oligomeric silsesquioxane (MA-POSS) onto the thiolated short quartz fibers (SQFs-SH) via the thiol-ene click chemistry. The resulting surface-functionalized fibers (P_xSQFs) exhibited tunable grafted layer thicknesses by controlling the thiol concentration, where P_0.33SQFs showed the roughest surface (Ra=17.92 nm) and the optimal grafted thickness (0.86 μm). All P_xSQFs were incorporated into the Bis-GMA-based matrix and photopolymerized by visible light to fabricate dental composites. Among all materials, the developed P_0.33SQFs-filled DRCs (P_0.33SQFs-DRCs) exhibited the highest flexural strength and modulus, fracture toughness, and fracture work, which were increased by 64.8, 123.3, 51.2, and 118.7%, respectively, over the unmodified SQFs-filled composites (p<0.05, n=6). Meanwhile, all-atom molecular dynamics (MD) simulations were conducted to elucidate the mechanical performance and interfacial behavior of P_xSQFs-DRCs, using the Gromacs-4.6.7 software package and a general AMBER force field. The results revealed that P_0.33SQFs-DRCs exhibited the strongest interfacial adhesion, the highest resistance during the fiber pull-out process, and the maximum stress response under both longitudinal and transverse uniaxial tension models. In vitro and in vivo cytocompatibility assessments confirmed that this P_0.33SQFs-DRCs material showed no adverse effects. This work provides a multiscale construction strategy for fiber surface functionalization and combines experimental and simulation studies on the interfacial behaviors of dental composites, which can offer a design guidance for the next-generation of dental materials with enhanced mechanical reliability and clinical safety.

Keywords

Fiber surface functionalization / Thiol-ene click reaction / Interfacial behaviors / Dental resin composites / Molecular dynamics simulations

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Funding

National Key Research and Development Program of China(2023YFB3809903/2023YFB3809900)

National Natural Science Foundation of China(52572297)

RIGHTS & PERMISSIONS

Donghua University, Shanghai, China