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儿茶酚化学启发的方法构建自交联聚合物纳米层作为多功能生物界面。

Catechol chemistry inspired approach to construct self-cross-linked polymer nanolayers as versatile biointerfaces.

机构信息

College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University , Chengdu 610065, China.

出版信息

Langmuir. 2014 Dec 16;30(49):14905-15. doi: 10.1021/la503872h. Epub 2014 Dec 3.

Abstract

In this study, we proposed a catechol chemistry inspired approach to construct surface self-cross-linked polymer nanolayers for the design of versatile biointerfaces. Several representative biofunctional polymers, P(SS-co-AA), P(SBMA-co-AA), P(EGMA-co-AA), P(VP-co-AA), and P(MTAC-co-AA), were first synthesized via reversible addition-fragmentation chain transfer (RAFT) polymerization, and then the catecholic molecules (dopamine, DA) were conjugated to the acrylic acid (AA) units by the facile carbodiimide chemistry. Then, the catechol (Cat) group conjugated biofunctional polymers, named PSS-Cat, PSBMA-Cat, PEGMA-Cat, PVP-Cat, and PMTAC-Cat, were applied for the construction of self-cross-linked nanolayers on polymeric substrates via the pH induced catechol cross-linking and immobilization. The XPS spectra, surface morphology, and wettability gave robust evidence that the catechol conjugated polymers were successfully coated, and the coated substrates possessed increased surface roughness and hydrophilicity. Furthermore, the systematic in vitro investigation of protein adsorption, platelet adhesion, activated partial thromboplastin time (APTT), thrombin time (TT), cell viability, and antibacterial ability confirmed that the coated nanolayers conferred the substrates with versatile biological performances. The PSS-Cat coated substrate had low blood component activation and excellent anticoagulant activity; while the PEGMA-Cat and PSBMA-Cat showed ideal resistance to protein fouling and inhibition of platelet activation. The PSS-Cat and PVP-Cat coated substrates exhibited promoted endothelial cell proliferation and viability. The PMTAC-Cat coated substrate showed an outstanding activity on bacterial inhibition. In conclusion, the catechol chemistry inspired approach allows the self-cross-linked nanolayers to be easily immobilized on polymeric substrates with the stable conformation and multiple biofunctionalities. It is expected that this low-cost and facile bioinspired coating system will present great potential in creating novel and versatile biointerfaces.

摘要

在这项研究中,我们提出了一种受儿茶酚化学启发的方法来构建表面自交联聚合物纳米层,以设计多功能生物界面。首先通过可逆加成-断裂链转移(RAFT)聚合合成了几种代表性的生物功能聚合物,P(SS-co-AA)、P(SBMA-co-AA)、P(EGMA-co-AA)、P(VP-co-AA)和 P(MTAC-co-AA),然后通过简单的碳二亚胺化学将儿茶酚(多巴胺,DA)接枝到丙烯酸(AA)单元上。然后,将儿茶酚(Cat)基团接枝的生物功能聚合物,命名为 PSS-Cat、PSBMA-Cat、PEGMA-Cat、PVP-Cat 和 PMTAC-Cat,通过 pH 诱导的儿茶酚交联和固定化应用于聚合物基底上的自交联纳米层的构建。XPS 光谱、表面形态和润湿性提供了有力的证据表明,儿茶酚接枝聚合物已成功涂覆,并且涂覆的基底具有增加的表面粗糙度和亲水性。此外,对蛋白质吸附、血小板黏附、活化部分凝血活酶时间(APTT)、凝血酶时间(TT)、细胞活力和抗菌能力的系统体外研究证实,涂覆的纳米层赋予了基底多功能的生物学性能。PSS-Cat 涂覆的基底具有低血液成分激活和优异的抗凝活性;而 PEGMA-Cat 和 PSBMA-Cat 则表现出理想的抗蛋白质污染和抑制血小板激活的能力。PSS-Cat 和 PVP-Cat 涂覆的基底表现出促进内皮细胞增殖和活力的能力。PMTAC-Cat 涂覆的基底对细菌抑制具有出色的活性。总之,儿茶酚化学启发的方法允许自交联纳米层以稳定的构象和多种生物功能轻松固定在聚合物基底上。预计这种低成本且简单的仿生涂层系统将在创造新型多功能生物界面方面具有巨大的潜力。

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