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Understanding the Effect of Hydration on the Bio-inert Properties of 2-Hydroxyethyl Methacrylate Copolymers with Small Amounts of Amino- or/and Fluorine-Containing Monomers
ACS Biomaterials Science & Engineering ( IF 5.8 ) Pub Date : 2020-04-01 , DOI: 10.1021/acsbiomaterials.0c00230
Ryohei Koguchi 1, 2 , Katja Jankova 3, 4 , Yuki Hayasaka 5 , Daisuke Kobayashi 5 , Yosuke Amino 5 , Tatsuya Miyajima 5 , Shingo Kobayashi 3 , Daiki Murakami 1, 3 , Kyoko Yamamoto 2 , Masaru Tanaka 1, 3
Affiliation  

Materials exhibiting “bio-inert properties” are essential for developing medical devices because they are less recognized as foreign substances by proteins and cells in the living body. We have reported that the presence of intermediate water (IW) with the water molecules loosely bound to a polymer is a useful index of the bio-inertness of materials. Here, we analyzed the hydration state and the responses to biomolecules of poly(2-hydroxyethyl methacrylate) (PHEMA) copolymers including small amounts of 2-(dimethylamino)ethyl methacrylate (DMAEMA) (N-series) or/and 2,2,2-trifluoroethyl methacrylate (TFEMA) (F-series). The hydration structure was analyzed by differential scanning calorimetry (DSC), the molecular mobility of the produced copolymers by temperature derivative of DSC (DDSC), and the water mobility by solid 1H pulse nuclear magnetic resonance (NMR). Although the homopolymers did not show bio-inert properties, the binary and ternary PHEMA copolymers with low comonomer contents showed higher bio-inert properties than those of PHEMA homopolymers. The hydration state of PHEMA was changed by introducing a small amount of comonomers. The mobility of both water molecules and hydrated polymers was changed in the N-series nonfreezing water (NFW) with the water molecules tightly bound to a polymer and was shifted to high-mobility IW and free water (FW) with the water molecules scarcely bound to a polymer. On the other hand, in the F-series, FW turned to IW and NFW. Additionally, a synergetic effect was postulated when both comonomers coexist in the copolymers of HEMA, which was expressed by widening the temperature range of cold crystallization, contributing to further improvement of the bio-inert properties.

中文翻译:

了解水合对少量氨基或/和含氟单体的甲基丙烯酸2-羟乙酯的生物惰性的影响

表现出“生物惰性”的材料对于开发医疗器械至关重要,因为它们很少被生物体内的蛋白质和细胞识别为异物。我们已经报道,中间水(IW)的水分子松散地结合到聚合物上是材料生物惰性的有用指标。在这里,我们分析了聚甲基丙烯酸2-羟乙酯(PHEMA)共聚物的水合状态和对生物分子的响应,其中包括少量的甲基丙烯酸2-(二甲氨基)乙酯(DMAEMA)(N系列)或/和2,2,甲基丙烯酸2-三氟乙基酯(TFEMA)(F系列)。通过差示扫描量热法(DSC)分析水合结构,通过DSC的温度导数(DDSC)分析制得的共聚物的分子迁移率,并通过固体1分析水的迁移率。H脉冲核磁共振(NMR)。尽管均聚物没有显示出生物惰性,但是具有低共聚单体含量的二元和三元PHEMA共聚物显示出比PHEMA均聚物更高的生物惰性。通过引入少量共聚单体可以改变PHEMA的水合状态。在水分子与聚合物紧密结合的N系列非冷冻水(NFW)中,水分子和水合聚合物的迁移率都发生了变化,而水分子几乎没有结合,则迁移为高迁移率IW和游离水(FW)聚合物。另一方面,在F系列中,FW转向IW和NFW。此外,当两种共聚单体共存于HEMA共聚物中时,可以推测出协同效应,这通过扩大冷结晶的温度范围来表示,
更新日期:2020-04-01
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