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Silk Fibroin-Substrate Interactions at Heterogeneous Nanocomposite Interfaces

机译：丝素蛋白-底物在异质纳米复合材料界面的相互作用。

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摘要

Silk fibroin adsorption at the heterogeneous hydrophobic-hydrophilic surface of graphene oxide (GO) with different degrees of oxidation is addressed experimentally and theoretically. Samples are prepared using various spin-assisted deposition conditions relevant to assembly of laminated nanocomposites from graphene-based components, and compared with silicon dioxide (SiO2) as a benchmark substrate. Secondary structure of silk backbones changes as a function of silk fibroin concentration, substrate chemical composition, and deposition dynamics are assessed and compared with molecular dynamic simulations. It is observed that protofibrils form at low concentrations while variance in the deposition speed has little effect on silk secondary structure and morphology. However, balance of nonbonded interactions between electrostatic and van der Waals contributions can lead to silk secondary structure retention on the GO surface. Molecular dynamics simulations of silk fibroin at different surfaces show that strong van der Waals interactions play a pivotal role in losing and disrupting secondary structure on graphene and SiO2 surfaces. Fine tuning silk fibroin structure on heterogeneous graphene-based surfaces paves the way toward development of biomolecular reinforcement for biopolymer-graphene laminated nanocomposites.
机译：实验和理论上解决了丝素蛋白在氧化程度不同的氧化石墨烯（GO）的疏水疏水疏水表面上的吸附问题。使用与自石墨烯基组分组装层压纳米复合材料有关的各种旋转辅助沉积条件制备样品，并与作为基准基材的二氧化硅（SiO2）进行比较。丝绸主链的二级结构随丝绸纤维蛋白浓度，底物化学组成和沉积动力学的变化而变化，并与分子动力学模拟进行比较。观察到原纤维在低浓度下形成，而沉积速度的变化对丝二级结构和形态几乎没有影响。但是，静电和范德华力之间非键相互作用的平衡会导致丝二级结构保留在GO表面。丝素蛋白在不同表面上的分子动力学模拟表明，强范德华相互作用在石墨烯和SiO2表面的二级结构丧失和破坏中起着关键作用。在异质石墨烯基表面上微调丝素蛋白结构为开发生物聚合物-石墨烯层压纳米复合材料的生物分子增强剂铺平了道路。

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  • 来源
    《Advanced Functional Materials》 |2016年第35期|6380-6392|共13页
  • 作者

    Grant Anise M.; Kim Ho Shin; Dupnock Trisha L.; Hu Kesong; Yingling Yaroslava G.; Tsukruk Vladimir V.;

  • 作者单位

    Georgia Inst Technol, Sch Mat Sci & Engn, Atlanta, GA 30332 USA;

    North Carolina State Univ, Dept Mat Sci & Engn, Raleigh, NC 27695 USA;

    North Carolina State Univ, Dept Mat Sci & Engn, Raleigh, NC 27695 USA;

    Georgia Inst Technol, Sch Mat Sci & Engn, Atlanta, GA 30332 USA;

    North Carolina State Univ, Dept Mat Sci & Engn, Raleigh, NC 27695 USA;

    Georgia Inst Technol, Sch Mat Sci & Engn, Atlanta, GA 30332 USA;

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