Understanding and Engineering the Nucleation of Enzyme Metal-Organic Frameworks

理解和设计酶金属有机框架的成核

• 批准号: 2102033
• 负责人: Joe Patterson
• 金额: $ 33.92万
• 依托单位: University of California-Irvine
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-07-15 至 2024-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2102033&HistoricalAwards=false
• 关键词: Understanding; Engineering; Nucleation; Enzyme; Metal

Enzymes are natural catalysts that can be used by chemical industries to speed up the rate of reactions and reduce the energy requirements of catalytic processes. However, enzymes are not typically stable outside of the physiological environment in which they evolved, significantly limiting their utility for industrial applications. A potential solution to this problem is to immobilize enzymes onto support structures. The ideal support material must be capable of loading high quantities of the active form of the enzyme. The support should also increase the stability and recyclability of the enzyme compared to the free enzyme in solution. Metal-organic frameworks (MOFs) are a promising class of materials for enzyme immobilization. MOFs are porous crystalline materials formed by the self-assembly of metal ions and organic ligands. Enzymes can be immobilized on MOFs by simply mixing the metal, ligand, and enzyme in aqueous solutions at room temperature. The enzymes are then incorporated into the MOF framework during the nucleation and growth processes. Understanding how this process works requires a detailed analysis of the system's nucleation and growth mechanisms. This fundamental mechanistic knowledge will provide robust design rules for the synthesis of enzyme-immobilized MOFs with high loading of the active form of the enzyme. The ability to immobilize practically any enzyme at the MOF surface has the potential to revolutionize the biotechnology industry and benefit society through lower energy chemical processes. The investigator will also develop a mobile K-12 outreach activity that uses low-cost microscopy to observe salt crystal growth. This project aims to determine the nucleation and growth mechanisms of enzyme MOF composite materials. The approach employs cryogenic and liquid-phase electron microscopy. Cryogenic electron microscopy will be used to trap intermediates and analyze their high-resolution structure. Liquid-phase electron microscopy will be used to monitor the kinetics of absorption, nucleation, and growth. The electron microscopy data will be supported by bulk scattering analysis using light and X-rays. The knowledge gained from these mechanistic studies will be used to re-engineer the interfacial chemistry to improve both encapsulation efficiency and enzymatic activity. The project will reveal the formation mechanisms, how the mechanisms can be manipulated by tuning the interfacial chemistry, and the structure-property relationships.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.

酶是天然催化剂，化学工业可以使用，以加快反应速度并降低催化过程的能量需求。但是，在它们进化的生理环境之外，酶通常并不是稳定的，从而大大限制了其用于工业应用的效用。解决此问题的潜在解决方案是将酶固定在支撑结构上。理想的支撑材料必须能够加载大量酶的活性形式。与溶液中的游离酶相比，支持还应提高酶的稳定性和可回收性。金属有机框架（MOF）是固定酶的有前途的材料类别。 MOF是由金属离子和有机配体的自组装形成的多孔晶体材料。可以通过在室温下将金属，配体和酶混合在水溶液中，将酶固定在MOF上。然后在成核和生长过程中将酶掺入MOF框架中。了解该过程的工作原理需要对系统的成核和生长机制进行详细分析。这种基本的机械知识将为合成酶的酶 - 弹性MOF的合成提供强大的设计规则，并具有高负载的酶的活性形式。 MOF表面实际上固定任何酶的能力有可能通过较低的能源化学过程彻底改变生物技术行业并使社会受益。研究人员还将开发一种移动的K-12外展活动，该活动使用低成本显微镜观察盐晶体的生长。该项目旨在确定酶MOF复合材料的成核和生长机制。该方法采用低温和液相电子显微镜。低温电子显微镜将用于捕获中间体并分析其高分辨率结构。液相电子显微镜将用于监测吸收，成核和生长的动力学。电子显微镜数据将通过使用光和X射线的散装散射分析来支持。从这些机械研究中获得的知识将用于重新设计界面化学，以提高封装效率和酶活性。该项目将揭示形成机制，如何通过调整界面化学来操纵机制以及结构性关系的关系。该奖项反映了NSF的法定任务，并被认为值得通过基金会的知识分子优点和更广泛的影响审查标准通过评估来进行评估。