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：Umit Ozkan研究所：俄亥俄州立大学建议编号：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)燃料电池中最显著的电位损失是由于阴极中的氧还原反应(ORR)动力学导致的事实，使得一些研究集中在开发新型ORR催化剂上。其中一些研究是基于自然启发的概念，即使用血红蛋白类型的分子来执行氧气还原功能。据报道，含有铁(Fe)或钴(Co)中心的大有机大环在高比表面积碳上负载时，对ORR具有活性。虽然这些复杂的化合物在燃料电池环境中不能长期稳定，但经过热处理后，剩余的含氮金属中心碳结构是活性和稳定的。尽管文献中有大量证据表明碳负载氮官能团(含金属中心和不含金属中心)作为潜在的PEM燃料电池阴极电催化剂可能具有氧还原活性，但对于活性中心的性质和氧还原反应的机理还没有清楚的了解。这项建议的重点是研究含氮碳纳米结构作为潜在的PEM燃料电池阴极催化剂的氧还原活性中心的性质。主要目标是(A)对活性中心的性质、金属中心的作用和碳载体结构有一个基本的了解，(B)开发这些催化剂的纳米合成技术，以及(C)建立一个知识库，以导致用作燃料电池电极的新型非贵金属催化材料的纳米级设计。虽然拟议研究的最终目标是开发新型的无铂PEM燃料电池电极，但目前的研究重点将放在合成含氮碳电极材料上，以具体研究和评估氧还原活性的影响因素，金属/氮官能团/碳纳米结构/氧还原活性之间的相互关系，负责活性的活性中心(S)，活性中心形成所需的前体材料的形式，以及这些材料在实际条件下的性能和稳定性。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，俄亥俄州立大学-IGERT项目的研讨会系列)，为研究生和本科生研究人员提供培训场地，以及创建演示工具，用于“女性工程新生迎新”项目，这些工具将激发人们的想象力，使她们对在工程领域的职业感到兴奋。该项目还将加强P.I.和法国CNRS催化研究所之间现有的国际合作。