Catalytic activity of nitrogen-containing functional groups supported on carbon structures for cathodic oxygen reduction reaction for PEM fuel cells

碳结构负载的含氮官能团对质子交换膜燃料电池阴极氧还原反应的催化活性

• 批准号: 0437451
• 负责人: Umit Ozkan
• 金额: --
• 依托单位: Ohio State University Research Foundation -DO NOT USE
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2005
• 资助国家: 美国
• 起止时间: 2005-01-01 至 2009-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=0437451&HistoricalAwards=false
• 关键词: Catalytic; activity; nitrogen; containing; functional

ABSTRACTPI: Umit OzkanInstitution: Ohio State UniversityProposal Number: 0437451ResearchThe high costs associated with the use of platinum (Pt) catalysts coupled with the fact that the most significant potential loss in polymer electrolyte membrane (PEM) fuel cells is due to the kinetics of the oxygen reduction reaction (ORR) in the cathode have led several studies to focus on the development of novel ORR catalysts. Some of these studies are based on the nature-inspired concept of using hemoglobin-type molecules to perform the oxygen reduction function. Large organic macrocycles containing iron (Fe) or cobalt (Co) centers are reported to be active for ORR when supported on high-surface area carbon. Although these complex compounds are not stable for long periods of time in the fuel cell environment, when they are subjected to a heat treatment, the remaining nitrogen-containing carbon structures with metal centers are shown to be active and stable.Although there is ample evidence in the literature about the possible oxygen reduction activity of carbon-supported nitrogen functional groups (with and without metal centers) as potential cathode electrocatalysts for PEM fuel cells, there is no clear understanding about the nature of active sites and the mechanism of oxygen reduction reaction. The focus of this proposal is investigation of the nature of oxygen reduction active sites in nitrogen containing carbon nano-structures as potential cathode catalysts for PEM fuel cells. The main objectives are (a) acquiring a fundamental understanding of the nature of active sites, the role of the metal centers and the carbon support structure, (b) developing techniques for nano-scale synthesis of these catalysts and (c) building a knowledge base that would lead to the nano-scale design of novel, non-precious metal catalytic materials to be used as fuel cell electrodes. While the ultimate goal of the proposed research is the development of novel, platinum-free PEM fuel cell electrodes, the present study will focus on the synthesis of nitrogen-containing carbon electrode materials to specifically study and assess the factors contributing to oxygen reduction activity, the inter-relation between metal/nitrogen functional groups/carbon nano-structure/oxygen reduction activity, the active site(s) responsible for activity, the forms of precursor material necessary for active site formation, and the performance and stability of these materials under real conditions.Broad ImpactThe move to a hydrogen economy is a national target - consequently the development of technologies that facilitate wide application of fuel cells are becoming increasingly important. The results of this work could bring the application of fuel cells closer to reality. Other impacts include curriculum development (new course in "Catalysis and Fuel Cells", seminar series in OSU-IGERT program), providing a training ground for graduate and undergraduate researchers, and creating demonstration tools to be used in the "Orientation for Women Engineering Freshmen" program that would capture the imagination and that would get them excited about a career in engineering. The project will also strengthen an existing international collaboration between the P.I. and the French CNRS-Catalysis Research Institute.

摘要PI：UMIT OzkaninStitution：俄亥俄州立大学培育编号：0437451研究与使用铂（PT）催化剂相关的高成本，以及聚合物电解质膜（PEM）燃料电池的最重要的潜在损失是由于氧化物的发展源（ORRE）的发展（ORR）的开发（ORR）的开发（ORR）的开发（ORR）的开发（ORR）的开发（催化剂。 其中一些研究基于自然启发的概念，即使用血红蛋白型分子执行还原功能。 据报道，在高表面区域碳上支撑时，含有铁（Fe）或钴（CO）中心的大型有机大环（Fe）或钴（CO）中心具有活性。 尽管这些复杂的化合物在燃料电池环境中长时间不稳定，但是当它们接受热处理时，剩余的含氮中心的含碳结构被证明是活跃且稳定的。细胞，对活性位点的性质和氧还原反应的机制没有明确的了解。该提案的重点是研究还原含碳纳米结构的氧气活性位点的性质，作为PEM燃料电池的潜在阴极催化剂。 主要目的是（a）获得对活性站点性质，金属中心和碳支持结构的性质的基本理解，（b）开发这些催化剂纳米级合成技术的技术，以及（c）建立一个知识基础，该知识基础将导致新型，非特殊的金属型型制度型燃料电池的纳米尺度设计。 While the ultimate goal of the proposed research is the development of novel, platinum-free PEM fuel cell electrodes, the present study will focus on the synthesis of nitrogen-containing carbon electrode materials to specifically study and assess the factors contributing to oxygen reduction activity, the inter-relation between metal/nitrogen functional groups/carbon nano-structure/oxygen reduction activity, the active site(s) responsible for activity, the forms of前体材料是主动地点形成所需的材料，以及在实际条件下这些材料的性能和稳定性。法线影响转向氢经济是一个国家目标 - 因此，发展有助于广泛应用燃料电池的技术的发展变得越来越重要。 这项工作的结果可能会使燃料电池的应用更接近现实。 其他影响包括课程开发（“催化和燃料电池”的新课程，OSU-IGERT计划中的研讨会系列），为研究生和本科研究人员提供培训理由，以及为“女性工程新生的方向使用”的示范工具，可以捕捉想象力，并使他们感到兴奋，这将使他们感到兴奋。 该项目还将加强P.I.之间现有的国际合作。和法国CNRS催化研究所。