Collaborative Research: Synthetic methane fixation cascades based on engineered membrane vesicles for biofuel cell applications

合作研究：基于工程膜囊泡的合成甲烷固定级联，用于生物燃料电池应用

• 批准号: 2221893
• 负责人: Wilfred Chen
• 金额: $ 25.11万
• 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: 2022
• 资助国家: 美国
• 起止时间: 2022-09-01 至 2026-02-28
• 项目状态: 未结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2221893&HistoricalAwards=false
• 关键词: Collaborative; Research; Synthetic; methane; fixation

Advances in oil and gas extraction techniques have made natural gas, composed primarily of methane, widely available for use. Large quantities of methane leak into the atmosphere during these operations. Well sites are often remote and isolated. Standard capture and treatment technologies are not generally feasible to apply in these cases. The objective of this project is to convert methane to electric power. Artificial enzyme cascades will be created to completely oxidize methane to CO2, generating electrons in the process. The electrons will be used in fuel cell applications. This project will include an education and outreach program that expands student access to project-based learning. Developing an integrated teaching, research, and curriculum development platform will engage graduate students, undergraduate, and high school students, particularly those in underrepresented groups.There is a big gap on converting mostly wasted methane to more valuable products under ambient temperature due to the lack of efficient enzyme cascades. To address this problem, the concept of fixing methane to methanol coupled to oxidation of methanol for electron release using an organized four-enzyme cascade on membrane vesicles is proposed. The membrane-bound enzyme found in methanotrophic bacteria will selectively convert methane to methanol under mild conditions. This is the foundation of the approach. Employing new hybrid enzyme-synthetic biology artificial enzyme cascades, using the enzyme-bound vesicles isolated directly from the host membranes, should completely oxidize methanol to CO2 and generate electrons for fuel-cell applications. Specifically, conjugating a protein scaffold onto the methane fixing enzyme-bound membrane vesicles will enable the assembly of three dehydrogenases for the sequential conversion of methane to carbon dioxide. Co-localization of the three dehydrogenases with the methane fixing enzyme will promote the synergistic action between the enzymes due to substrate channeling, resulting in an enhancement in the overall current density. One added benefit of cascading the enzymes is to enable the improved transfer of NADH and NAD+ between dehydrogenase and the methane fixing enzyme for higher catalytic efficiency. The expected result is a new platform to generate synthetic membrane vesicles system for methane fixation to CO2 to power biofuel cells, and to serve as a technology platform for other membrane-bound enzyme systems.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.

石油和天然气提取技术的进步使天然气成为主要由甲烷组成的天然气，广泛可供使用。在这些操作过程中，大量甲烷泄漏到大气中。井站点通常是遥远和孤立的。在这些情况下，标准捕获和治疗技术通常不可行。 该项目的目的是将甲烷转换为电力。 将创建人工酶级联反应以将甲烷完全氧化为CO2，从而在此过程中产生电子。电子将用于燃料电池应用。 该项目将包括一个教育和外展计划，该计划扩大学生对基于项目的学习的访问。开发一个综合的教学，研究和课程发展平台将吸引研究生，本科生和高中生，尤其是那些人数不足的学生。由于缺乏有效的酶级联，在环境温度下大多将浪费的甲烷转换为更有价值的产品的差距很大。为了解决这个问题，提出了将甲烷固定在甲醇与甲醇偶联的甲醇偶联以进行电子释放的概念，该概念使用有组织的四酶级联反应在膜囊泡上释放。在轻度条件下，发现甲烷菌细菌中发现的膜结合的酶将有选择地将甲烷转化为甲醇。这是方法的基础。使用直接从宿主膜中分离的酶结合的囊泡采用新的杂化酶合成生物学人工酶级联反应，应将甲醇完全氧化为CO2并为燃料细胞应用产生电子。具体而言，将蛋白质支架偶联到甲烷固定酶结合的膜囊泡上将使三种脱氢酶的组装以将甲烷转化为甲烷向二氧化碳的顺序转化。三种脱氢酶与甲烷固定酶的共定位将促进由于底物通道引起的酶之间的协同作用，从而导致总体电流密度的增强。级联酶的一个额外好处是，脱氢酶和甲烷固定酶之间的NADH和NAD+的转移可以提高催化效率。预期的结果是一个新的平台，以生成合成膜囊泡系统，以固定二氧化碳，以供电生物燃料细胞，并用作其他膜结合酶系统的技术平台。这项奖项反映了NSF的法定任务，并通过评估该基金会的知识点功能和广泛的影响来评估NSF的法定任务，并被认为是值得的。