Mechanical Unfolding of Network Nodes Drives the Stress Response of Protein-Based Materials.

IF 15.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY ACS Nano Pub Date : 2024-11-02 DOI:10.1021/acsnano.4c07352
Joel Nowitzke, Sanam Bista, Sadia Raman, Narayan Dahal, Guillaume Stirnemann, Ionel Popa
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Abstract

Biomaterials synthesized from cross-linked folded proteins have untapped potential for biocompatible, resilient, and responsive implementations, but face challenges due to costly molecular refinement and limited understanding of their mechanical response. Under a stress vector, these materials combine the gel-like response of cross-linked networks with the mechanical unfolding and extension of proteins from well-defined 3D structures to unstructured polypeptides. Yet the nanoscale dynamics governing their viscoelastic response remains poorly understood. This lack of understanding is further exacerbated by the fact that the mechanical stability of protein domains depends not only on their structure, but also on the direction of the force vector. To this end, here we propose a coarse-grained network model based on the physical characteristics of polyproteins and combine it with the mechanical unfolding response of protein domains, obtained from single molecule measurements and steered molecular dynamics simulations, to explain the macroscopic response of protein-based materials to a stress vector. We find that domains are about 10-fold more stable when force is applied along their end-to-end coordinate than along the other tethering geometries that are possible inside the biomaterial. As such, the macroscopic response of protein-based materials is mainly driven by the unfolding of the node-domains and rearrangement of these nodes inside the material. The predictions from our models are then confirmed experimentally using force-clamp rheometry. This model is a critical step toward developing protein-based materials with predictable response and that can enable applications for shape memory and energy storage and dissipation.

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网络节点的机械展开驱动蛋白基材料的应力响应
由交联折叠蛋白质合成的生物材料在生物相容性、弹性和响应性方面具有尚未开发的潜力,但由于分子精细化成本高昂以及对其机械响应的了解有限而面临挑战。在应力矢量作用下,这些材料将交联网络的凝胶状反应与蛋白质从明确定义的三维结构到非结构多肽的机械展开和延伸结合在一起。然而,人们对其粘弹性响应的纳米级动力学特性仍然知之甚少。蛋白质结构域的机械稳定性不仅取决于其结构,还取决于力矢量的方向,这一事实进一步加剧了人们的这种认识不足。为此,我们提出了一个基于多聚蛋白质物理特性的粗粒度网络模型,并将其与单分子测量和定向分子动力学模拟获得的蛋白质结构域的机械展开响应相结合,来解释基于蛋白质的材料对应力矢量的宏观响应。我们发现,与生物材料内部可能存在的其他系留几何形状相比,沿端到端坐标施力时,结构域的稳定性要高出约 10 倍。因此,蛋白质材料的宏观响应主要是由材料内部节点域的展开和这些节点的重新排列驱动的。我们的模型预测结果随后通过力钳流变仪得到了实验证实。该模型是开发具有可预测响应的蛋白质基材料的关键一步,可用于形状记忆、能量存储和耗散。
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来源期刊
ACS Nano
ACS Nano 工程技术-材料科学:综合
CiteScore
26.00
自引率
4.10%
发文量
1627
审稿时长
1.7 months
期刊介绍: ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.
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