Crosslinking Polymer Brushes with Ethylene Glycol-Containing Segments: Influence on Physicochemical and Antifouling Properties
Crosslinking Polymer Brushes with Ethylene Glycol-Containing Segments: Influence on Physicochemical and Antifouling Properties
复制标题
DOI：
10.1021/acs.langmuir.6b02958
复制
发表时间：
2016-10-11
期刊：
影响因子：
3.9
通讯作者：
Benetti, Edmond M.
中科院分区：
文献类型：
--
作者：
Dehghani, Ella S.;Spencer, Nicholas D.;Benetti, Edmond M.
在聚甲基丙烯酸羟乙酯（PHEMA）刷中引入不同类型和浓度的交联会影响它们的界面、物理化学性质，最终控制它们对蛋白质的吸附。以HEMA为原料，采用表面引发原子转移自由基聚合（SI-ATRP）方法，分别添加二（乙二醇）二甲基丙烯酸酯（DEGDMA）和四（乙二醇）二甲基丙烯酸酯（TEGDMA）作为交联剂和不添加交联剂，合成了PHEMA刷和刷水凝胶。线性（纯PHEMA）刷具有高水合性和低模量，另外还提供了有效的非特异性蛋白质吸附屏障。相比之下，刷子-水凝胶更硬，水化程度更低，交联的存在影响了熵驱动的构象屏障，阻碍了生物分子与刷子的表面相互作用。这导致蛋白质在低浓度的短交联下的物理吸附。在较高的DEGDMA含量或较长的tegdma基交联存在下，由于较高浓度的乙二醇（EG）单元增加了界面水缔合，刷状水凝胶恢复了其防污性能。
The introduction of different types and concentrations of crosslinks within poly(hydroxyethyl methacrylate) (PHEMA) brushes influences their interfacial, physicochemical properties, ultimately governing their adsorption of proteins. PHEMA brushes and brush-hydrogels were synthesized by surface-initiated, atom-transfer radical polymerization (SI-ATRP) from HEMA, with and without the addition of di(ethylene glycol) dimethacrylate (DEGDMA) or tetra (ethylene glycol) dimethacrylate (TEGDMA) as crosslinkers. Linear (pure PHEMA) brushes show high hydration and low modulus and additionally provide an efficient barrier against nonspecific protein adsorption. In contrast, brush-hydrogels are stiffer and less hydrated, and the presence of crosslinks affects the entropy-driven, conformational barrier that hinders the surface interaction of biomolecules with brushes. This leads to the physisorption of proteins at low concentrations of short crosslinks. At higher contents of DEGDMA or in the presence of longer TEGDMA-based crosslinks, brush-hydrogels recover their antifouling properties due to the increase in interfacial water association by the higher concentration of ethylene glycol (EG) units.