高分子胺功能化三维结构Pd基金属纳米晶的氧还原性能研究

项目名称： 高分子胺功能化三维结构Pd基金属纳米晶的氧还原性能研究

项目编号： No.21473111

项目类型： 面上项目

立项/批准年度： 2015

项目学科： 数理科学和化学

项目作者： 陈煜

作者单位： 陕西师范大学

项目金额： 85万元

中文摘要： 氧还原反应(ORR)是直接醇类燃料电池中重要反应之一。三维结构贵金属纳米晶对ORR呈现出高的电催化活性和稳定性。传统上，ORR活性改进研究主要集中在调控贵金属纳米晶的尺寸、形貌和化学组成。近来，通过贵金属纳米粒子表面化学功能化来改进其电催化性能成为一个全新的电催化剂设计理念。本项目拟在高分子胺类化合物(PMA)体系中合成具有各种形貌、尺寸和组成的PMA功能化三维结构Pd基金属纳米晶。揭示溶液pH、反应温度、还原剂类型、PMA分子构型等实验参数对产物形貌、结构、尺寸、组成的影响，深入掌握PMA在Pd基金属纳米晶合成过程的功能及作用机制。利用电化学技术研究PMA功能化Pd基金属纳米晶对ORR的电催化性能。结合光谱数据研究Pd基金属纳米晶表面PMA吸附层改进电催化活性、稳定性和耐醇性的关键机理。本项目对于Pd基金属纳米晶合成基础研究、发展新的电催化设计理念等方面具有很好的理论和实践意义。

中文关键词： 钯；高分子胺；表面化学功能化；三维结构；氧还原反应

英文摘要： The electrocatalytic oxygen reduction reaction (ORR) is one of the key reactions in direct alcohol fuel cells. In general, three-dimensionally (3D) interconnected noble metal nanostructures exhibit superior electrocatalytic activity and durability towards the ORR because of their attractive structural features, such as porosity, high surface area, interconnected nanostructure, excellent electrical connectivity, and high density of twinned defects. Traditionally, ORR improvement mainly focus on the design and manipulation of the composition, particle size and shape of noble metal nanostructures. Very recently, a new trend in electrocatalyst designs has been proposed, which is based on the modification of the metal surface by nonmetallic molecules that can block the adsorption of poisoning species and spectator anions. In the project, we report a convenient wet chemical method to synthesize the polymeric amine (PMA) functionalized 3D Pd-based nanostructures with controlled morphology, size and composition. In the process, the influence of experimental parameters (such as the reaction temperature, reaction time, solution pH and molecular structure, etc.) on the size, morphology and composition of Pd-based nanostructures will be investigated systemically. Furthermore, the electrocatalytic activity, durability and alcohol tolerant ability of PMA functionalized 3D Pd-based nanostructures towards the ORR will be explored by using various electrochemical techniques. In addition, the effect of PMA layer adsorbed on 3D Pd-based nanostructures surface on electrocatalytic activity, stability and alcohol tolerant ability of 3D Pd-based nanostructures also will be demonstrated detailedly by analyzing experimental data. In summary, the implementation of the project will favor the fundamental research of 3D Pd-based nanostructures synthesis and the development of new electrocatalyst designs.

英文关键词： Palladium;Polymeric amine;Surface chemical modification;Three-dimensional structure;Oxygen reduction reaction