Collaborative Research: Organized Nanochannel Materials from Biomolecular Magnetic Organic Frameworks-

非技术描述在溶液的纳米级过滤过程中生物分子成分的受控传输对于精细化学、药物研究、药物输送以及其他复杂的纯化和材料制造过程中的许多应用来说是一项至关重要的任务。到目前为止，纸基材料的随机形态和糟糕的孔隙率已经严重阻碍了生物分子的传输和催化现象的定制。目前的生物衍生和合成材料具有随机的多孔形态，具有广泛的官能度和孔隙率，这影响了它们的有效分子传输和生物催化活性，特别是与对映体生物化合物的关系。因此，需要更深入地了解具有长程有序低维结构元素的潜在的强韧和柔性膜，以促进新型纳米孔生物衍生材料的基础知识，其中包括具有受控和响应的通道组织的新型开孔组织材料。为此，我们建议使用具有明确的选择性相互作用能力的多肽片段，包括手性相关的转运和磁性团簇/原子，以协调开放单元细胞与分子孔尺寸。此外，还可以利用外加磁场来创造更大规模的响应材料，其传输特性受其方向和强度的影响。实验研究将由机器学习和计算方法指导和协助。最后，该研究项目将为具有不同实验和计算生物材料科学背景的研究生和本科生提供跨学科的培训，用于先进材料和生物分子产业。这项建议将考虑新型有序纳米通道生物分子纳米材料，以了解具有增强的孔洞尺寸和拓扑控制的高效有序凝胶状自适应材料的设计原理，材料和能量传输，手性生物分子的选择和存储/释放，以及未来的手性生物催化模板。为了建立低缺陷生物-金属-有机骨架(MOF)的组装原则，必须解决许多关键问题，例如由于非常短的多肽序列、小孔尺寸、有限的对称性以及用于定向和响应加载、运输或对映体选择和生物催化能力的潜在的缺陷而导致的单元尺寸和孔有限的问题。该团队将合成、设计和研究的主要新颖单元是基于生物编码肽的生物分子磁性有机骨架(BiMOF)，这些肽具有金属结合的末端基团，用于与磁性离子/簇配位。需要解决的关键基本问题是如何引入功能生物分子元素的引导共组装作为一种工具，用于定向构建具有稳定和精确控制的孔尺寸、通道拓扑、连续性和手性的形态以及自适应的离子和质量/能量传输性质的大规模有组织的分级材料。不同对称性和维度的生物编码磁性生物骨架单元细胞和生物分子晶体的设计将通过与定制的单元细胞参数、孔尺寸、通道尺寸、磁矩构型、孔和微晶体稳定性以及具有生物分子选择性和手性的大孔的重组能力的特定位置的金属肽配合来探索。实验工作将以理论、机器学习和大规模分子模拟为指导，以了解潜在的科学原理。这项拟议的研究将利用多尺度建模和机器学习，以实验验证为动力，为设计和组装具有固有重新配置能力的健壮但自适应的纳米通道BiMOF架构开发“特定于技术”的规则。这项工作可以加强对纳米晶体和纳米片远程有序组装的有序多相纳米材料中复杂输运现象的基本理解。最后，PI的迷你工作坊系列：生活和职业将通过与应邀访问母校的前学生和博士后互动来促进学生的准备，这些学生和博士后在工业、国家实验室和学术界拥有成功的职业生涯。该项目将提供实验、计算和数据科学工具的集成教学；具体地说，基于项目的模块将被设计并纳入高级课程并通过NanHUB分发。该项目由材料研究部门(DMR)的生物材料(BMAT)和金属和金属纳米结构(MMN)计划联合资助。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 descriptionControlled transport of biomolecular ingredients during nanoscale filtration of solutions is a vital task for many applications in fine chemistry, pharmaceutical research, drug delivery, and other sophisticated purification and materials making processes. To date, random morphologies and poorly controlled porosity of paper-based materials have significantly prevented tailoring biomolecular transport and catalytic phenomena. Current bio-derived and synthetic materials possess random porous morphologies with wide distributions of functionalities and porosities that compromise their effective molecular transport and biocatalytic activity, especially in relationship to enantiotropic biological compounds. Therefore, deeper understanding of potentially strong and flexible membranes with long-range ordered low-dimensional structural elements is required to advance the fundamental knowledge of novel nanoporous bio-derived materials with inclusion of novel open pore organized materials with controlled and responsive channel organization. For this purpose, we suggest using peptide segments with well-defined ability for selective interactions including chiral-related transport and magnetic clusters/atoms for coordination of open unit cells with molecular pore dimensions. Moreover, external magnetic field can be explored to create larger-scale responsive materials with transport properties directed by its direction and strength. Experimental research will be guided and assisted by machine learning and computational approaches. Finally, the research project will provide interdisciplinary training to graduate and undergraduate students with diverse backgrounds in experimental and computational biomaterials science for advanced material and biomolecular industry.Technical descriptionThis proposal will consider novel classes of organized nanochannel biomolecular nanomaterials for understanding the design principles of efficient organized gel-like adaptive materials with enhanced porosity dimension and topological control, materials and energy transport, chiral biomolecules selection and storage/release, and prospective chiral biocatalytic templates. Numerous critical issues must be addressed in order to establish principles of assembly of low-defect bio-metal-organic frameworks (MOFs) such as problems with limited unit sizes and pores due to the very short peptide sequences, small pore sizes, limited symmetries achievable, and high concentration of defects for directional and responsive loading, transport or potential for enantiotropic selection and biocatalytical abilities. The major novel units that the team will synthesize, design, and study are biomolecular magnetic organic frameworks (BiMOFs) based upon biologically encoded peptides with metal-binding terminal groups for coordination with magnetic ions/clusters. The key fundamental question to be addressed is how the guided co-assembly of functional biomolecular elements can be introduced as a tool for directed construction of large-scale organized hierarchical materials with stable and precisely controlled morphology of pore dimensions, channel topology, continuity, and chirality, and adaptive ionic and mass/energy transport properties. Design of biologically encoded magnetic bio-framework unit cells and biomolecular crystals of different symmetries and dimensions will be explored via site-specific metal-peptide coordination with tailored unit cell parameters, pore dimensions, channel dimensionalities, magnetic moment configuration, pores and microcrystal stability, and restructuring abilities of large-sized pores with biomolecular selectivity and chirality. The experimental work will be guided by theory, machine learning, and large-scale molecular simulations to understand the underlying scientific principles. The proposed research will leverage multi-scale modeling and machine learning powered by experimental verification to develop “technology-specific” rules for the design and assembly of robust but adaptive nanochannel BiMOF architectures with inherent ability to reconfigure. The work can enhance fundamental understanding of complex trasport phenomena in organized multi-phase nanomaterials with long-range organized assembly of nanocrystals and nanosheets. Finally, the PI’s mini-workshops Homecoming Series: Life and Career will be used to facilitate student readiness by interacting with former students and post-docs invited to visit their alma mater who enjoy successful careers in industry, national labs, and academia. This project will provide teaching the integration of experimental, computational, and data science tools; specifically, project-based modules will be designed and incorporated into upper-level courses and distributed through nanoHUB.This project is jointly funded by the Biomaterials (BMAT) and the Metals and Metallic Nanostructures (MMN) Programs of the Division of Materials Research (DMR).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.