R&D Center for Membrane Technology and Department of Chemical Engineering , Chung Yuan Christian University , Chungli District , Taoyuan 320 , Taiwan , R.O.C.
Laboratoire de Génie Chimique , Université Paul Sabatier , 118 Route de Narbonne , 31062 Toulouse , Cedex 9 , France.
Langmuir. 2019 Feb 5;35(5):1909-1918. doi: 10.1021/acs.langmuir.8b02483. Epub 2018 Oct 29.
Hydrogels are hydrated networks of flexible polymers with versatile biomedical applications, and their resistance to nonspecific protein adsorption is critical. On the other hand, functionalization with other biomacromolecules would greatly enhance their biotechnological potential. The aim of this research is to prepare low fouling hydrogel polymers for selective protein immobilization. Initially, hydrogels were prepared by controlling the composition ratios of 2-carboxyethyl acrylate (CA) and 2-dimethylaminoethyl methacrylate (DMAEMA) monomers in an N, N-methylene-bis-acrylamide (NMBA) cross-linked free radical polymerization reaction. This series of hydrogels (C1D9 to C9D1) were then analyzed by X-ray photoelectron spectroscopy (XPS) and dynamic laser scattering to confirm the actual polymer ratios and surface charge. When the composition ratio was set at CA:6 vs DMEAMA:4 (C6D4), the hydrogel showed nearly neutral surface charge and an equivalent reaction ratio of CA vs DMAEMA in the hydrogel. Subsequent analysis showed excellent antifouling properties, low blood cell adhesion, hemocompatibility, and platelet deactivation. Moreover, this hydrogel exhibited pH responsiveness to protein adsorption and was then used to facilitate the immobilization of lipase as an indication of active protein functionalization while still maintaining a low fouling status. In summary, a mixed-charge nonfouling pseudozwitterionic hydrogel could be prepared, and its pH-responsive adsorption holds potential for designing a biocompatible tissue engineering matrix or membrane enzyme reactors.
水凝胶是具有多种生物医学应用的柔性聚合物的水合网络，其对非特异性蛋白质吸附的抵抗力至关重要。另一方面，与其他生物大分子的功能化将极大地提高其生物技术潜力。本研究旨在制备低污染水凝胶聚合物以进行选择性蛋白质固定化。最初，通过控制 2-羧乙基丙烯酰胺（CA）和 2-二甲氨基乙基甲基丙烯酸酯（DMAEMA）单体在 N，N-亚甲基双丙烯酰胺（NMBA）交联自由基聚合反应中的组成比来制备水凝胶。然后通过 X 射线光电子能谱（XPS）和动态激光散射分析对一系列水凝胶（C1D9 至 C9D1）进行分析，以确认实际聚合物比和表面电荷。当组成比设置为 CA：6 与 DMEAMA：4（C6D4）时，水凝胶表现出近中性表面电荷和水凝胶中 CA 与 DMAEMA 的当量反应比。随后的分析表明其具有出色的抗污染性能，低血细胞黏附性，血液相容性和血小板失活作用。此外，该水凝胶对蛋白质吸附具有 pH 响应性，随后用于促进脂肪酶的固定化，作为活性蛋白质功能化的指示，同时仍保持低污染状态。综上所述，可以制备混合电荷的非污染假两性离子水凝胶，其 pH 响应性吸附有望用于设计生物相容的组织工程基质或膜酶反应器。
