通用粘合剂中的丙烯酰胺单体。
Acrylamide monomers in universal adhesives.
机构信息
KU Leuven (University of Leuven), Department of Oral Health Sciences, BIOMAT & UZ Leuven (University Hospitals Leuven), Dentistry, Leuven, Belgium; Tanta University, Department of Dental Biomaterials, Tanta, Egypt.
National Institute of Advanced Industrial Science and Technology (AIST), Health and Medical Research Institute, Takamatsu, Japan; Okayama University, Graduate School of Medicine, Dentistry and Pharmaceutical Sciences, Department of Pathology & Experimental Medicine, Okayama, Japan.
出版信息
Dent Mater. 2023 Mar;39(3):246-259. doi: 10.1016/j.dental.2023.01.003. Epub 2023 Jan 27.
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.
目的
单官能单体 2-羟乙基甲基丙烯酸酯（HEMA）通常添加到通用胶粘剂（UA）中以改善表面润湿性并防止相分离。然而，HEMA 促进了胶粘剂界面的吸水和水解，从而影响了对牙本质的长期粘结。本研究探讨了两种丙烯酰胺单体是否可以替代在蚀刻和冲洗（2E&R）和自酸蚀（1SE）粘结模式下应用的 UA 配方中的 HEMA。
方法
将四种实验性 UA 粘结到牙本质的磨切表面。除了 12wt%10-MDP、25wt%Bis-GMA 和 10wt%TEGDMA 作为常见单体组成、20wt%乙醇和 15wt%水作为溶剂以及 3wt%聚合相关添加剂外，四种配方仅在作为 TEGDMA 替代品和 HEMA 替代品的丙烯酰胺交联单体“FAM-201”、作为 HEMA 替代品的羟乙基丙烯酰胺单体“HEAA”、含有 HEMA 的配方（“HEMA+”）或不含 HEMA 的对照配方（“HEMA-”）中仅使用 15wt%浓度的 15wt%水。该劈裂牙研究设计涉及在一侧牙半部分应用 2E&R 模式，在相应的半部分应用 1SE 模式。一半的微样本的微拉伸粘结强度在一周的蒸馏水储存后进行测量（“即时”1w μTBS），另一半在额外的 6 个月储存后进行测量（“老化”6m μTBS）。统计分析采用线性混合效应（LME）模型（p<0.05）。此外，还进行了界面 TEM 表征、薄膜（TF）XRD 表面分析、LogP 测定和细胞毒性测定。
结果
当在 E&R 和 SE 粘结模式下均应用时，FAM-201 的 μTBS 在 1w 和 6m 时均显著高于 HEMA+。当在 SE 模式下应用时，HEAA 的 μTBS 在 1w 时显著低于 HEMA+。TF-XRD 和 TEM 显示出相似的化学和超微结构界面特征，包括稳定的 10-MDP_Ca 盐纳米层。FAM-201 的细胞毒性最低，LogP 居中，而 HEAA 的 LogP 最高，表明其具有较高的亲水性和吸水敏感性。
意义
丙烯酰胺共聚单体 FAM-201 可以替代 UA 配方中的 HEMA，而 HEAA 则不能。
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