Rational Design of Hydrogel Polymer Nanoparticles Based on a Receptor Recognition Mechanism of Endotoxin and Its Application in Endotoxin Removal

IF 4.4 2区 化学 Q2 MATERIALS SCIENCE, MULTIDISCIPLINARY
Zihao Wan, Yunli Yu, Qiaolian Cheng, Weicheng Tang, Wenfeng Tan and Mingming Liu*, 
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Abstract

Endotoxins, also known as lipopolysaccharides (LPS), are common exogenous pyrogens with notable pathogenic properties. The removal of endotoxins from water is essential due to the potential health hazards posed by exposure to bacterial or cyanobacterial endotoxins. Herein, we report an abiotic affinity material, a hydrogel polymer nanoparticle (HNP) as a potential absorbent for endotoxin removal. The polymer affinity ligand was discovered via a combination of rational design and directed evolution. Under the guidance of an endotoxin–receptor recognition mechanism, several receptor-like hydrogel polymer nanoparticle libraries were rationally created by incorporating candidate monomers with functionalities complementary either to the negatively charged phosphate groups or the hydrophobic fatty acid chains in endotoxin structure. MArg-HNP 4 that has high affinity, rapid kinetics, pH-responsivity, and broad-spectrum selectivity to LPS derivatives was identified by directed evolution, namely, multiple rounds of library construction and affinity screening. The screened MArg-HNP 4 was then in situ polymerized on the surface of SiO2 to prepare adsorption columns for the removal of endotoxin from water. The homemade column has LPS removal efficacy comparable to that packed with commercial ToxinEraser resin modified with polymyxin B. It also exhibits excellent regeneration performance, favorable biological safety, high cost-effectiveness, facile chemical synthesis, and high stability and robustness. These attributes make SiO2@MArg-HNP 4 a promising alternative to existing commercial endotoxin removal columns.

Abstract Image

基于内毒素受体识别机制的水凝胶聚合物纳米颗粒的合理设计及其在内毒素去除中的应用
内毒素,也称为脂多糖(LPS),是一种常见的外源性热原,具有显著的致病性。由于暴露于细菌或蓝藻内毒素所造成的潜在健康危害,从水中去除内毒素是必不可少的。在此,我们报道了一种非生物亲和材料,水凝胶聚合物纳米颗粒(HNP)作为去除内毒素的潜在吸收剂。通过合理设计和定向进化的结合,发现了聚合物亲和配体。在内毒素受体识别机制的指导下,通过引入与内毒素结构中带负电荷的磷酸基团或疏水脂肪酸链功能互补的候选单体,合理构建了多个类受体水凝胶聚合物纳米粒子文库。通过定向进化,即多轮文库构建和亲和筛选,鉴定出对LPS衍生物具有高亲和力、快速动力学、ph响应性和广谱选择性的mar - hnp4。将筛选的marg - hnp4原位聚合在SiO2表面,制备吸附柱,用于去除水中的内毒素。自制色谱柱的LPS去除效果可与多粘菌素b改性的商用ToxinEraser树脂填料相媲美,再生性能优异,生物安全性好,成本效益高,化学合成简便,稳定性和鲁棒性高。这些特性使SiO2@MArg-HNP 4成为现有商业内毒素去除柱的有希望的替代品。
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来源期刊
CiteScore
7.20
自引率
6.00%
发文量
810
期刊介绍: ACS Applied Polymer Materials is an interdisciplinary journal publishing original research covering all aspects of engineering, chemistry, physics, and biology relevant to applications of polymers. The journal is devoted to reports of new and original experimental and theoretical research of an applied nature that integrates fundamental knowledge in the areas of materials, engineering, physics, bioscience, polymer science and chemistry into important polymer applications. The journal is specifically interested in work that addresses relationships among structure, processing, morphology, chemistry, properties, and function as well as work that provide insights into mechanisms critical to the performance of the polymer for applications.
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