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蛋白质排斥型抗凝血混合电荷纤维素衍生物涂层。

Protein repellent anti-coagulative mixed-charged cellulose derivative coatings.

机构信息

Laboratory for Characterization and Processing of Polymers (LCPP), Faculty of Mechanical Engineering, University of Maribor, Maribor, Slovenia.

Institute for Chemistry and Technology of Biobased Systems, Graz University of Technology, Stremayrgasse 9, A-8010, Graz, Austria.

出版信息

Carbohydr Polym. 2021 Feb 15;254:117437. doi: 10.1016/j.carbpol.2020.117437. Epub 2020 Nov 25.

Abstract

This study describes the formation of cellulose based polyelectrolyte charge complexes on the surface of biodegradable polycaprolactone (PCL) thin films. Anionic sulphated cellulose (CS) and protonated cationic amino cellulose (AC) were used to form these complexes with a layer-by-layer coating technique. Both polyelectrolytes were analyzed by charge titration methods to elucidate their pH-value dependent protonation behavior. A quartz crystal microbalance with dissipation (QCM-D) in combination with X-ray photoelectron spectroscopy (XPS) and atomic force microscopy (AFM) were used to follow the growth, stability and water content of up to three AC/CS bi-layers in aqueous environment. This was combined with coagulation studies on one, two and three bilayers of AC/CS, measuring the thrombin formation rate and the total coagulation time of citrated blood plasma with QCM-D. Stable mixed charged bilayers could be prepared on PCL and significantly higher masses of AC than of CS were present in these complexes. Strong hydration due to the presence of ammonium and sulphate substituents on the backbone of cellulose led to a significant BSA repellent character of three bilayers of AC/CS coatings. The total plasma coagulation time was increased in comparison to neat PCL, indicating an anticoagulative nature of the coatings. Surprisingly, a coating solely composed of an AC layer significantly prolonged the total coagulation time on the surfaces although it did not prevent fibrinogen deposition. It is suggested that these cellulose derivative-based coatings can therefore be used to prevent unwanted BSA deposition and fibrin clot formation on PCL to foster its biomedical application.

摘要

本研究描述了在可生物降解的聚己内酯(PCL)薄膜表面上形成基于纤维素的聚电解质电荷复合物。阴离子硫酸化纤维素(CS)和质子化阳离子氨基纤维素(AC)被用于通过层层涂层技术形成这些复合物。两种聚电解质都通过电荷滴定法进行分析,以阐明其 pH 值依赖性质子化行为。使用带有耗散的石英晶体微天平(QCM-D)结合 X 射线光电子能谱(XPS)和原子力显微镜(AFM),可以跟踪在水环境中多达三层 AC/CS 双层的生长、稳定性和含水量。这与在 AC/CS 的一层、两层和三层上进行的凝聚研究相结合,通过 QCM-D 测量凝血酶形成率和柠檬酸化血浆的总凝血时间。可以在 PCL 上制备稳定的混合带电双层,并且这些复合物中存在的 AC 量明显高于 CS。由于纤维素主链上存在铵和硫酸盐取代基,强烈的水合作用导致 AC/CS 三层涂层具有明显的 BSA 排斥特性。与纯 PCL 相比,总血浆凝固时间增加,表明涂层具有抗凝血性质。令人惊讶的是,尽管 AC 层的涂层不能防止纤维蛋白原沉积,但它显著延长了表面的总凝血时间。因此,这些基于纤维素衍生物的涂层可用于防止 PCL 上不必要的 BSA 沉积和纤维蛋白凝块形成,从而促进其在生物医学中的应用。

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