Department of Chemical and Biomolecular Engineering, University of California Berkeley, Berkeley, California 94720, United States.
Department of Bioengineering, University of California, Berkeley, California 94720, United States.
Biomacromolecules. 2024 Jan 8;25(1):328-337. doi: 10.1021/acs.biomac.3c01002. Epub 2023 Dec 5.
Protein brushes not only play a key role in the functionality of neurofilaments but also have wide applications in biomedical materials. Here, we investigate the effect of ionic strength on the morphology of protein brushes using continuous-space self-consistent field theory. A coarse-grained multiblock charged macromolecular model is developed to capture the chemical identity of amino acid sequences. For neurofilament heavy (NFH) brushes at pH 2.4, we predict three morphological regimes: swollen brushes, condensed brushes, and coexisting brushes, which consist of both a dense inner layer and a diffuse outer layer. The brush height predicted by our theory is in good agreement with the experimental data for a wide range of ionic strengths. The dramatic height decrease is a result of the electrostatic screening-induced transition from the overlapping state to the isolated state of the coexisting brushes. We also studied the evolution of the scattering and mechanical responses accompanying the morphological change. The oscillation in the reflectivity spectra characterizes the existence and microstructure of the inner condensed layer, whereas the shoulder in the force spectra signifies a swollen morphology.
蛋白质刷不仅在神经丝的功能中起着关键作用,而且在生物医学材料中也有广泛的应用。在这里,我们使用连续空间自洽场理论研究离子强度对蛋白质刷形态的影响。开发了一种粗粒多嵌段带电高分子模型来捕捉氨基酸序列的化学特性。对于 pH 值为 2.4 的神经丝重链 (NFH) 刷,我们预测了三种形态状态:溶胀刷、凝聚刷和共存刷,它们由密集的内层和弥散的外层组成。我们的理论预测的刷高与广泛的离子强度范围内的实验数据非常吻合。由于静电屏蔽诱导的共存刷从重叠状态到隔离状态的转变,刷高急剧下降。我们还研究了伴随形态变化的散射和力学响应的演变。反射率谱中的振荡特征在于内层凝聚层的存在和微观结构,而力谱中的肩状特征则表明刷的溶胀形态。