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.

0967988施密特克燃料电池通过阳极的氧化反应和阴极的还原反应将化学能直接转化为电能。在酶生物燃料电池中，传统的燃料电池催化剂（例如Pt、Pd、Ru）在阳极处被燃料氧化酶（例如葡萄糖氧化酶、醇脱氢酶、果糖脱氢酶）和在阴极处被氧还原酶（例如漆酶、胆红素氧化酶）替代。目前，酶生物燃料电池的主要局限性是功率输出低和寿命有限。俄克拉荷马州诺曼校区的首席研究员大卫·施密特克（David Schmidtke）和丹尼尔·格拉茨霍弗（Daniel Glatzhofer）对限制因素进行了假设。在酶促生物燃料电池中，大多数酶的氧化还原中心被埋在蛋白质壳中，并且电不可接近。因此，大多数氧化还原酶通常不与电极交换电子。他们提出通过合成氧化还原聚合物来增加酶生物燃料电池的功率输出，该氧化还原聚合物增加氧化还原酶和电极之间的电子转移速率（即电流）。这些新颖的基于PEI的氧化还原聚合物通过有效地收集和穿梭于酶的氧化还原中心和电极表面之间的电子来产生高电流。这些聚合物含有连接到聚合物的金属物质，二茂铁化合物。调整系统将需要合成具有不同长度间隔臂的聚合物。PI的目标是将功率输出提高20-200倍。酶生物燃料电池不会解决国家的能源需求。然而，随着对便携式能源的需求增加，发展了对替代的可再生能源的需求。酶生物燃料电池是一种有吸引力的能量转换技术，因为它们在20 -40？并且消耗底物，例如在生物系统中容易获得的糖。由于其固有的选择性，基于酶的阳极和阴极可以在相同的隔室中操作而无需分离膜，从而减小尺寸和重量。它们具有用于体内（例如起搏器、可植入传感器）和离体（例如远程位置感测、移动的电子器件）系统的潜在应用。研究人员打算利用他们的研究作为一种工具，以增加该领域对潜在学生的吸引力。他们的信念，基于研究，是一个学生对科学的态度和他在科学方面的成就提高与实践经验。为了帮助增加学生继续学习科学和工程的可能性，建议的教育活动与研究机会包括本科生的研究机会和代表性不足的群体的夏季研究实习，与中学教师的研究机会相匹配。