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首页> 外文期刊>Applied Surface Science >Biomimetic PDMS-hydroxyurethane terminated with catecholic moieties for chemical grafting on transition metal oxide-based surfaces
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Biomimetic PDMS-hydroxyurethane terminated with catecholic moieties for chemical grafting on transition metal oxide-based surfaces

机译：仿生PDMS-羟基氨基甲酸酯，端基为端基，用于在过渡金属氧化物基表面上进行化学接枝

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The aim of this work was to synthesize a non-isocyanate poly(dimethylsiloxane) hydroxyurethane with biomimetic terminal catechol moieties, as a candidate for inorganic and metallic surface modification. Such surface modifier is capable to strongly attach onto metallic and inorganic substrates forming layers and, in addition, providing water-repellent surfaces. The non-isocyanate route is based on carbon dioxide cycloaddition into bis-epoxide, resulting in a precursor bis(cyclic carbonate)-polydimethylsiloxane(CCPDMS), thus fully replacing isocyanate in the manufacture process. A biomimetic approach was chosen with the molecular composition being inspired by terminal peptides present in adhesive proteins of mussels, like Mefp (Mytilus edulis foot protein), which bear catechol moieties and are strong adhesives even under natural and saline water. The catechol terminal groups were grafted by aminolysis reaction into a polydimethylsiloxane backbone. The product, PDMSUr-Dopamine, presented high affinity towards inhomogeneous alloy surfaces terminated by native oxide layers as demonstrated by quartz crystal microbalance (QCM-D), as well as stability against desorption by rinsing with ethanol. As revealed by QCM-D, X-ray photoelectron spectroscopy (XPS) and computational studies, the thickness and composition of the resulting nanolayers indicated an attachment of PDMSUr-Dopamine molecules to the substrate through both terminal catechol groups, with the adsorbate exposing the hydrophobic PDMS backbone. This hypothesis was investigated by classical molecular dynamic simulation (MD) of pure PDMSUr-Dopamine molecules on SiO2 surfaces. The computationally obtained PDMSUr-Dopamine assembly is in agreement with the conclusions from the experiments regarding the conformation of PDMSUr-Dopamine towards the surface. The tendency of the terminal catechol groups to approach the surface is in agreement with proposed model for the attachment PDMSUr-Dopamine. Remarkably, the versatile PDMSUr-Dopamine modifier facilitates such functionalization for various substrates such as titanium alloy, steel and ceramic surfaces. (C) 2017 Elsevier B.V. All rights reserved.
机译：这项工作的目的是合成具有仿生末端邻苯二酚部分的非异氰酸酯聚（二甲基硅氧烷）羟基氨基甲酸酯，作为无机和金属表面改性的候选物。这种表面改性剂能够牢固地附着在形成层的金属和无机基底上，并且另外提供疏水表面。非异氰酸酯途径是基于将二氧化碳环加成到双环氧化物中，从而生成前体双（环状碳酸酯）-聚二甲基硅氧烷（CCPDMS），从而在制造过程中完全替代异氰酸酯。选择了一种仿生方法，其分子组成受到贻贝黏附蛋白（例如Mefp（紫草足蛋白））中存在的末端肽的启发，后者具有邻苯二酚部分，即使在天然和盐水中也具有很强的黏附力。通过氨基分解反应将邻苯二酚端基接枝到聚二甲基硅氧烷主链中。 PDMSUr-多巴胺产品对由天然氧化物层终止的非均质合金表面表现出高亲和力，如石英晶体微天平（QCM-D）所证明的那样，以及对乙醇冲洗解吸的稳定性。如QCM-D，X射线光电子能谱（XPS）和计算研究所揭示的，所得纳米层的厚度和组成表明PDMSUr-多巴胺分子通过两个末端邻苯二酚基团与底物连接，而被吸附物暴露了疏水性。 PDMS主干。通过经典的分子动力学模拟（MD）对SiO2表面上的纯PDMSUr-多巴胺分子进行了研究。通过计算获得的PDMSUr-多巴胺组装体与关于PDMSUr-多巴胺朝向表面构象的实验结论相符。末端邻苯二酚基团趋向表面的趋势与所提出的附着PDMSUr-多巴胺的模型一致。值得注意的是，通用的PDMSUr-多巴胺改性剂可促进各种基材（例如钛合金，钢和陶瓷表面）的功能化。 （C）2017 Elsevier B.V.保留所有权利。

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