RUI: Collaborative Research: Understanding the protein-polysaccharide interactions of natural composite materials in one and two dimensions

非技术性总结生物大分子是生命所必需的大分子，如蛋白质、碳水化合物、脂类和核酸。所有的生物体都是由各种生物大分子组成的，因此，了解它们的分子相互作用对于预测生物材料的形态、结构和功能是至关重要的。生物复合材料中蛋白质-多糖相互作用的研究对从医学到环境科学和材料科学等领域都具有重要意义。从自然界中使用的各种生物复合材料中可以看出，这些材料的用途非常广泛。然而，为了促进在现代技术中部署新的生物复合材料，需要开发新的方法来调整这些材料的性能以适应特定的技术需求。操纵分子形成具有精确控制、大小、间距和形状的分层结构的能力是该项目的中心目标，以便能够从单一结构快速制造多层结构。此外，该项目将为高中生和本科生提供研究、培训和教育机会，以更好地了解生物材料科学和生物大分子的分子相互作用。拟议的研究将与南泽西州本科生和K-12 STEM教育项目的需求无缝结合，这将特别有利于具有工程、化学、物理、生物和计算机科学背景的学生，他们必须在毕业前进行研究。此外，这项提议将使其他研究人员能够使用开发的工具和路线图来再生具有关键功能和可定制选项的生物复合材料。技术综述丝素和角蛋白等天然生物大分子代表结构蛋白质，而纤维素代表多糖。了解它们的分子相互作用对于释放一系列新材料、彻底改变我们制造多结构和多功能系统的方式至关重要。到目前为止，关于各种生物大分子的形态如何组装仍然缺乏知识，我们也不了解它们的相互作用如何决定物理化学性质。将分子间和分子内的形态修饰联系起来，将提供对分子自组装如何进展以及时空形态如何控制结构和物理化学性质的基本理解。达到这一水平的理解和控制将是导致制造坚固的多层次结构生物复合材料(如2D薄膜和1D纤维)的能力的关键。它还将有助于预测蛋白质二级结构与碳水化合物结晶度之间的关系，从而为细胞机械传感、细胞再生、膜分离、隔热和能量生产创造潜在的应用。本项目假设由离子液体再生的蛋白质-多糖生物复合材料的物理化学和形态性质主要受蛋白质二级结构、基于葡萄糖的微晶和生物大分子主链到主链插层的形成和尺寸的调节。为了解决这一假设，将追求两个主要目标，包括：i)作为分子结构和加工条件的函数的蛋白质-多糖材料的表征；ii)了解蛋白质二级结构和纤维素结晶度与材料的链插层、形态和机械稳定性之间的关系。该奖项反映了NSF的法定使命，并通过使用基金会的智力优势和更广泛的影响审查标准进行评估，被认为值得支持。

NON-TECHNICAL SUMMARYBiological macromolecules are large molecules which are fundamentally necessary for life such as proteins, carbohydrates, lipids, and nucleic acids. All organisms are composed of a variety of these biomacromolecules, and as such, understanding their molecular interactions is essential for predicting morphology, structure, and function of biomaterials. The study of protein-polysaccharide interactions in biocomposite materials carries implications for fields ranging from medicine to environmental science and materials science. These materials are extremely versatile as shown from a variety of biocomposites used in nature. However, to facilitate deployment of new biocomposite materials in modern technology, the development of new methodologies is required to tune the properties of these materials to suit specific technological demands. The ability to manipulate molecules to form hierarchical structures with precise control, size, spacing, and shape is a central objective of this project in order to enable the rapid fabrication of multi-level structures from single structures. In addition, this project will provide research, training and educational opportunities to high school and undergraduate students for a better understanding of biomaterials science and molecular interactions of biological macromolecules. The proposed research will be seamlessly associated with the needs of the South Jersey undergraduate and K-12 STEM education programs, which will be particularly beneficial for students of engineering, chemistry, physics, biology and computer science backgrounds who are required to undertake research for graduation. Furthermore, this proposal will enable other researchers to use the developed tools and roadmaps for the regeneration of biocomposite materials with critical functionalities and customizable options. TECHNICAL SUMMARYNatural biomacromolecules such as silk and keratin represent structural proteins, while cellulose represents polysaccharides. Understanding their molecular interactions is critical for unleashing a flora of new materials, revolutionizing the way we fabricate multi-structural and multi-functional systems. Knowledge to date is still lacking on how the morphology of various biomacromolecules assemble nor do we understand how their interactions dictate physicochemical properties. Linking morphology modification at the inter- and intra-molecular levels will provide a basic understanding of how the molecular self-assembly progresses and how spatiotemporal morphologies control the structure and physicochemical properties. Achieving this level of understanding and control will be crucial for progress leading to the ability to fabricate robust multi-level structural biocomposites such as 2D films and 1D fibers. It will also help to predict the relationship between protein secondary structures and carbohydrate crystallinity, thus creating potential applications for cellular mechanosensing, cellular regeneration, membrane separation, thermal insulation and energy production. This project hypothesizes that the physicochemical and morphological properties of protein-polysaccharide biocomposites regenerated from ionic liquids are mainly regulated by the formation and dimension of protein secondary structures, glucose-based crystallites, and biomacromolecules backbone-to-backbone chain intercalations. Two main objectives will be pursued to address this hypothesis, including, i) the characterization of protein-polysaccharide materials as a function of molecular structures and processing conditions; ii) understand the relationship between protein secondary structure and cellulose crystallinity in relation to chain intercalation, morphology, and mechanical stability of materials.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.