Polyethylenimine Redox Polymers for Bioelectrocatalysis

用于生物电催化的聚乙烯亚胺氧化还原聚合物

• 批准号: 0967988
• 负责人: David Schmidtke
• 金额: $ 32.73万
• 依托单位: University of Oklahoma Norman Campus
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2010
• 资助国家: 美国
• 起止时间: 2010-07-01 至 2014-06-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0967988&HistoricalAwards=false
• 关键词: Polyethylenimine; Redox; Polymers; Bioelectrocatalysis

0967988SchmidtkeFuel cells convert chemical energy directly into electricity through an oxidation reaction at the anode and a reduction reaction at the cathode. In enzymatic biofuel cells, traditional fuel cell catalysts (e.g. Pt, Pd, Ru) are replaced by fuel oxidizing enzymes (e.g. Glucose Oxidase,Alcohol Dehydrogenase, Fructose Dehydrogenase) at the anode and oxygen reducing enzymes (e.g. Laccase, Bilirubin Oxidase) at the cathode. Currently the main limitations of enzymatic biofuel cells are low power output and limited lifetimes. Principal Investigators David Schmidtke and Daniel Glatzhofer at the University of Oklahoma, Norman Campus have hypothesized on the limiting factors. In enzymatic biofuel cells, the redox center of most enzymes is buried in the protein shell and electrically inaccessible. Thus most redox enzymes do not normally exchange electrons with an electrode. They propose to increase the power output of enzymatic biofuel cells by synthesizing redox polymers that increase the rate of electron transfer (i.e. current flow)between the redox enzymes and electrodes. These novel PEI-based redox polymers produce high currents by efficiently collecting and shuttling electrons between the enzyme¡¦s redox center and the electrode surface. These polymers contain metal species, ferrocene compounds, linked to the polymer. Tuning the system will require synthesis of polymers with different lengths of spacer arms. The PIs are targeting a 20-200 fold improvement in power output. Enzymatic biofuel cells will not solve the nation¡¦s energy needs. However, as the demand for portable energy increases, there develops a need for alternative renewable energy sources. Enzymatic biofuel cells are an attractive energy conversion technology because they operate at mild temperatures of20-40?aC and under neutral pH and consume substrates such as sugars that are readily available in biological systems. Because of their inherent selectivities, enzyme based anodes and cathodes can operate in the same compartment without separating membranes thereby reducing size and weight. They have potential applications for both in vivo (e.g. pacemakers, implantable sensors) and ex vivo (e.g. remote site sensing, mobile electronics) systems. The investigators intend to use their research as a vehicle to increase the attractiveness of the field to potential students. Their belief, based on studies, is that a student¡¦s attitude toward science and his achievement in science improves with hands-on experiences. To help increase the likelihood that students will continue their studies in science and engineering, proposed educational activities with research opportunities include Research Opportunities for Undergraduate students and Summer Research Internships for Underrepresented Groups, matched with Research Opportunities for Middle School Teachers.

0967988SCHMIDTKEFUEL细胞通过阳极处的氧化反应和阴极的还原反应直接转化化学能。在酶生物燃料细胞中，传统的燃料电池催化剂（例如PT，PD，RU）被燃料氧化酶（例如葡萄糖氧化酶，葡萄糖氧化酶，酒精脱氢酶，果糖脱氢酶）在阳极和氧气减少酶（例如，均质酶，bilirirubin氧化酶）的ACTACHOPAPASED。目前，酶促生物燃料细胞的主要局限性是低功率输出和有限的寿命。俄克拉荷马大学诺曼校区的首席调查员戴维·施密特克（David Schmidtke）和丹尼尔·格拉茨霍夫（Daniel Glatzhofer）假设了限制因素。在酶促的生物燃料细胞中，大多数酶的氧化还原中心都建在蛋白质壳中，并无法接近电。大多数氧化还原酶通常不会与电子交换电子。他们建议通过合成氧化还原聚合物来增加氧化还原酶和电极之间的电子转移速率（即电流流）来增加酶生物燃料细胞的功率输出。这些新型的基于PEI的氧化还原聚合物通过有效收集和穿梭电子在酶氧化还原中心和电极表面之间产生高电流。这些聚合物含有与聚合物相关的金属物种，二茂二烯化合物。调整系统将需要合成具有不同长度的间隔臂的聚合物。 PI的目标是动力输出的20-200倍。酶生物燃料细胞不会解决国家的能源需求。但是，随着对便携式能源的需求增加，需要替代可再生能源。酶促生物燃料细胞是一种有吸引力的能量转化技术，因为它们在20-40？ac的轻度温度下运行，在中性pH值下进行，并且消耗了诸如生物系统中易于使用的糖基质。由于其继承选择性，基于酶的阳极和阴极可以在同一隔室中运行，而无需分开机制，从而减小了尺寸和重量。它们在体内（例如起搏器，可植入传感器）和Ex Vivo（例如远程站点敏感性，移动电子）系统都有潜在的应用。调查人员打算将他们的研究用作工具，以提高该领域对潜在学生的吸引力。他们基于研究的信念是，学生对科学的态度及其在科学方面的成就可以通过动手经验改善。为了帮助增加学生在科学和工程领域的研究的可能性，提出的具有研究机会的教育活动包括针对本科生的研究机会和为代表性不足的小组提供的夏季研究实习，并与中学教师的研究机会相匹配。