Evaluation of a photo-initiated copper(I)-catalyzed azide-alkyne cycloaddition polymer network with improved water stability and high mechanical performance as an ester-free dental restorative
Evaluation of a photo-initiated copper(I)-catalyzed azide-alkyne cycloaddition polymer network with improved water stability and high mechanical performance as an ester-free dental restorative
复制标题
光引发铜（I）催化叠氮-炔环加成聚合物网络的评估，作为无酯牙科修复剂，该聚合物网络具有改善的水稳定性和高机械性能
DOI：
10.1016/j.dental.2021.08.010
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发表时间：
2021
期刊：
影响因子：
5
通讯作者：
Bowman, Christopher N.
中科院分区：
文献类型：
--
作者：
Wang, Xiance;Gao, Guangzhe;Song, Han Byul;Zhang, Xinpeng;Stansbury, Jeffrey W.;Bowman, Christopher N.
目的是开发和表征与普通BisGMA/TEGDMA（70/30）树脂相比具有高机械性能、低聚合诱导应力的无酯醚基光-CuAAC树脂，方法合成了以三苯基乙烷为中心的醚连接的三叠氮单体，并与醚连接的三叠氮单体共光聚合。在可见光照射下，使用铜（II）预催化剂和CQ/EDAB作为引发剂，研究了醚基CuAAC配方的热机械性能、聚合动力学和收缩应力以及相对于常规BisGMA/TEGDMA（70/30）牙科树脂的弯曲性能。结果与BisGMA/TEGDMA（70/30）树脂相比，醚基CuAAC网络（AK/AZ-1）的玻璃化转变温度稍低，但其水稳定性较好（108 ° C vs 128 °C），但由于其更尖锐的玻璃化转变，AK/AZ-1 CuAAC网络在高达100 °C下保持高于1 GPa的储能模量。此外，与BisGMA/TEGDMA网络相比，醚基AK/AZ-1网络表现出降低的收缩应力（0.56 MPavs1.0 MPa）和高得多的弯曲韧性（7.6 MJ/m3 vs1.6 MJ/m3），同时显示出略低的弯曲模量和略高的弯曲强度。此外，委员会认为，醚基AK/AZ-1 CuAAC网络显示出与BisGMA/TEGDMA网络相当的水稳定性，具有略高的吸水性（46 μg/mm 3 vs 38 μg/mm 3）和更低的水溶性（2.3 μg/mm 3 vs4.4 μg/mm 3）。显著性与先前开发的氨基甲酸酯相比，采用基于醚的疏水CuAAC制剂显著改善了CuAAC网络的水稳定性。基于CuAAC网络。此外，与常规使用的BisGMA/TEGDMA制剂相比，醚基CuAAC网络的降低的收缩应力、相当的弯曲强度/弯曲模量和优异的上级弯曲韧性使其成为目前广泛使用的甲基丙烯酸酯基牙科清洁剂的有希望的无酯替代品。
ObjectiveThe objective is to develop and characterize an ester-free ether-based photo-CuAAC resin with high mechanical performance, low polymerization-induced stress compared with common BisGMA/TEGDMA (70/30) resins, and improved water stability in comparison to previously developed urethane-based photo-CuAAC resins.MethodsTriphenyl-ethane-centered ether-linked tri-azide monomers were synthesized and co-photopolymerized with ether-linked tri-alkyne monomers under visible light irradiation using a copper(II) pre-catalyst and CQ/EDAB as the initiator. The ether-based CuAAC formulation was investigated for thermo-mechanical properties, polymerization kinetics and shrinkage stress, and flexural properties with respect to a conventional BisGMA/TEGDMA (70/30) dental resin. In addition, both the ether-based CuAAC resin and the urethane-based CuAAC resin were examined for their water stability using the BisGMA/TEGDMA (70/30) resin as a control.ResultsThe ether-based CuAAC network (AK/AZ-1) exhibited a slightly lower glass-transition temperature compared with the BisGMA/TEGDMA network (108 °Cvs128 °C), but because of its much sharper glass transition, the AK/AZ-1 CuAAC-network maintained storage modulus higher than 1 GPa up to 100 °C. In addition, the ether-based AK/AZ-1 network exhibited reduced shrinkage stress (0.56 MPavs1.0 MPa) and much higher flexural toughness (7.6 MJ/m3vs1.6 MJ/m3) while showing slightly lower flexural modulus and slightly higher flexural strength compared with the BisGMA/TEGDMA network. Moreover, the ether-based AK/AZ-1 CuAAC network displayed comparable water stability in comparison to the BisGMA/TEGDMA network with slightly higher water sorption (46 μg/mm3vs38 μg/mm3) and much lower water solubility (2.3 μg/mm3vs4.4 μg/mm3).SignificanceEmploying the ether-based hydrophobic CuAAC formulation significantly improved the water stability of the CuAAC network compared with previously developed urethane-based CuAAC networks. Furthermore, compared with the conventionally used BisGMA/TEGDMA formulation, the reduced shrinkage stress, comparable flexural strength/flexural modulus, and the superior flexural toughness of the ether-based CuAAC network make it a promising ester-free alternative to the currently widely-used methacrylate-based dental restoratives.