基于碳纳米管/石墨烯杂化材料的一体式氧还原电极可控构筑

The purposes of this project are to develop a method for controllable assembly of carbon nanotube/graphene monolith and explore its potential as a directly used oxygen reduction electrode in fuel cells or metal/air batteries. In our previous research, we found that tuning the electronic structure of carbon materials could improve the oxygen reduction activity. The performance of gas diffusion electrode was affected by the aggregation and additive content which may obstacle the electronic transfer and mass diffusion process. The controllable construction of monolith electrode should be a good solution to these problems. This project will study the controllable preparation of a monolith electrode, and the pore structure, conductivity and mechanical property will be optimized to enhance oxygen reduction reaction process. On the basis of these investigations, the combination of electronic structure tuning and nano-architecture construction will be studied. Finally, we will investigate the practical application of this monolith electrode in fuel cells or metal/air batteries. This project will provide a new route for monolith electrode preparation and property control. The researches of this project will promote the theory studies on resolving the electrode process of oxygen reduction reaction and accelerate the real application of nanocarbon materials in function-directed design and controllable assembly field.

本项目旨在研究基于碳纳米管/石墨烯杂化材料的一体式氧还原电极可控构筑，探索该一体式电极在燃料电池或金属/空气电池中的应用。前期研究发现对碳质纳米材料的电子结构进行调控可以提高其氧还原反应活性，但是制备的气体扩散电极受材料分散状态、辅助组分等的影响，其导电与传质过程受到阻碍，性能大大降低。直接制备具有可控结构的宏观一体式电极可能是一条有效解决上述问题的途径。本项目重点研究利用碳纳米管/石墨烯杂化材料构筑一体式电极，通过调控其孔结构、导电性、机械性能等性质优化其氧还原反应过程；研究电子结构调控与一体式电极构筑的过程耦合；研究该电极独自作为氧还原电极在燃料电池或金属/空气电池中的应用前景。本项目的实施为利用纳米工程方法制备一体电极、调控其性质提供新思路，对氧还原电极过程的解析具有重要的理论指导意义，在基于碳质纳米材料的功能导向材料设计和可控组装方面具有实际应用价值。

本项目研究了基于碳纳米管/石墨烯杂化材料的一体式氧还原电极可控构筑，探索了该一体式电极在直接甲醇燃料电池或锂空气电池中的应用。在本项目中，我们利用氧化和刻蚀方法实现了多壁碳纳米管的可控剥离，制备了碳纳米管/石墨烯杂化材料。同时利用杂原子掺杂改变了其电子结构，提高了氧还原活性；利用贵金属铂复合制备了高性能氧还原催化剂。本项目制备得到的一体式电极在直接甲醇燃料电池和锂空气电池中表现出良好的性能。此外我们还利用上述方法制备了层次孔碳材料和碳气凝胶材料，这些材料在电化学储能领域也表现出优异的性能。本项目制备的具有可控结构宏观一体式电极在保障氧还原反应活性同时，可以有效改善气体扩散电极材料分散状态、辅助组分聚集等问题，有利于降低欧姆极化和传质极化。本项目为利用纳米工程方法的制备一体电极、调控其性质提供新思路，对氧还原电极性能提升具有促进作用，未来在基于碳质纳米材料的功能导向材料设计和可控组装方面具有实际应用价值。