Collaborative Proposal: DNA guided assembly of enzyme cascades for biocatalytic fuel cell applications

合作提案：用于生物催化燃料电池应用的 DNA 引导酶级联组装

• 批准号: 1263774
• 负责人: Wilfred Chen
• 金额: $ 41万
• 依托单位: University of Delaware
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2013
• 资助国家: 美国
• 起止时间: 2013-08-01 至 2017-07-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1263774&HistoricalAwards=false
• 关键词: Collaborative; Proposal; DNA; guided; assembly

Enzymatic fuel cells have received considerable attention because of their potential for direct conversion of abundant raw materials to electricity. The use of multi-enzyme cascades is particularly attractive as they offer the possibility of achieving a higher current density by the sequential oxidization of fuels. However, efficient substrate and electron channeling are two of the most important bottlenecks in improving the power output of multi-enzyme fuel cells. An award from the National Science Foundation Catalysis & Biocatalysis Program to Professors Wilfred Chen of the University of Delaware and Nosang Myung of the University of California-Riverside will support investigation of approaches to surmount these obstacles. The overall objective of this proposal is to investigate the use of a genetically controlled, DNA-based modular scaffold approach for the spatially-defined self-assembly of a multi-enzyme cascade for enhanced substrate and electron channeling. A simple and scalable electrospinning method will be developed to synthesize nanofiber mat electrodes with a very high surface area. A genetically designed mediator will then connect the assembly to the mat electrode. The modular nature of the proposed design allows easy alteration of spacing between the enzymes, mediators and the electrodes for investigating the optimal substrate and electron channeling in a rational manner. The unique combination of nanoengineering and bioengineering approaches will enable Chen and Myung to systematically investigate the factors affecting the overall performance of the multi-enzyme fuel cell. The initial testing of the concept will be demonstrated for the conversion of cellulose to gluconic acid, with other reactions to be studied subsequently.The proposed research is scientifically significant because the concept is built on ideas from biology extending to an entirely new engineering application. Because of the modular nature of the design, it is anticipated that the proposed framework will have a huge impact on the assembly of other multi-enzyme cascades. The proposed methodology will provide a future platform useful for the self-assembly of a wide range of multienzyme systems for fuel cell applications. From an educational perspective, graduate students participating in this research will gain an integrated perspective of the important interfaces and synergies connecting biochemistry, electrochemistry, and nanotechnology. The PIs plan outreach programs through the Mathematics Engineering Science Achievement Program at UC Riverside and the establishment of a Homeschoolers Day program in Delaware.

酶燃料电池因其将大量原料直接转化为电能的潜力而受到广泛关注。多酶级联的使用特别有吸引力，因为它们提供了通过燃料的顺序氧化获得更高电流密度的可能性。然而，有效的底物和电子通道是提高多酶燃料电池功率输出的两个最重要的瓶颈。美国国家科学基金会催化与生物催化项目向特拉华大学的Wilfred Chen教授和加州大学河滨分校的Nosang Myung教授颁发了一项奖项，以支持对克服这些障碍的方法的研究。本提案的总体目标是研究使用一种遗传控制的，基于dna的模块化支架方法，用于多酶级联的空间定义自组装，以增强底物和电子通道。将开发一种简单、可扩展的静电纺丝方法来合成具有非常高表面积的纳米纤维垫电极。然后，一个基因设计的介质将把组装物连接到垫子电极上。所提出的设计的模块化性质使得酶、介质和电极之间的间距可以很容易地改变，从而以合理的方式研究最佳底物和电子通道。纳米工程和生物工程方法的独特结合将使Chen和Myung能够系统地研究影响多酶燃料电池整体性能的因素。该概念的初步测试将用于纤维素转化为葡萄糖酸，随后将研究其他反应。这项提议的研究在科学上具有重要意义，因为这个概念是建立在从生物学延伸到一个全新的工程应用的思想之上的。由于设计的模块化性质，预计所提出的框架将对其他多酶级联的组装产生巨大影响。所提出的方法将为燃料电池应用中广泛的多酶系统的自组装提供一个有用的未来平台。从教育的角度来看，参与这项研究的研究生将获得一个综合的视角，了解生物化学、电化学和纳米技术之间的重要界面和协同作用。pi计划通过加州大学河滨分校的数学工程科学成就计划和在特拉华州建立一个家庭学校日计划来推广项目。