低维碳材料于纳米结构衬底上的组装调控及超级电容器选择性构建研究

Low-dimensional carbon material (carbon nanotube, Graphene-class nanoplates) is one of the most promising electrode materials for next-generation supercapacitors. However, the intrinsic outstanding electrochemical activity has not been fully utilized at the current state-of-the-art of high frequency- and high energy- supercapacitors, since the assembly strategies of low-dimensional carbon materials on the current collectors in a controllable way are still scarce, and the underlying mechanism of inter-connection assembly of low-dimensional carbon materials in the electrode fabrication is even not clear. To overcome the challenge, this project proposes a study on regulated assembly of low-dimensional carbon materials, synergistically guided by nano-structured templates grown on current collectors and the loaded transition metal catalysts. A systematic study on the assembly behavior and assembly mechanism of carbon nano-units affected by the configuration of nano-structured templates and the distribution pattern of metal catalysts. On the basis of the summarization and derivation, the intrinsic relationship of (1) Assembly mode and packing density of low-dimensional materials-(2) Electrode mass loading of active materials-(3) Internal pore structures and pore size distribution of monolith carbon electrodes-(4) High frequency performance of supercapacitors-(5) Energy density of supercapacitors, the applicability of the involved carbon electrodes obtained at different assembly conditions is evaluated, and then an electrode design criterion for selective construction of specific supercapacitors (high frequency supercapacitor or high energy supercapacitor ) is proposed, which can provide both the theoretical and technical guidance on performance improvement for supercapacitors.

低维碳材料（碳纳米管、石墨烯纳米片）是最具应用前景的下一代超级电容器电极材料之一，但是在现有高频型、高能型超级电容器的应用研究中并未能充分发挥其固有的高电化学活性，受限于缺乏在集流体上施行可控原位组装低维碳材料的有效方法及对低维碳材料接合组装生长机理的认知。针对该问题，申请项目提出采用集流体衬底上构建的纳米结构模板结合所负载的过渡金属催化剂协同调控低维碳材料原位生长及组装的研究思路，系统考察碳纳米材料单元在纳米结构衬底构型和催化剂分布调控的协同影响下的组装行为和组装机理。在总结与归纳低维碳材料组装方式、密度-电极活性材料载量-整体式电极内部孔道结构和孔径分布特征-超级电容器频率响应特性-超级电容器储能密度之间内在联系的基础上，评估不同组装调控条件下所获电极对于不同类属超级电容器需求的适用性，提出超级电容器选择性构建的指导性判据，为高频型、高能型超级电容器的性能优化提供理论与技术指导。

低维碳材料（碳纳米管、石墨烯纳米片）是最具应用前景的下一代超级电容器电极材料之一，但是在现有高频型、高能型超级电容器的应用研究中并未能充分发挥其固有的高电化学活性，受限于缺乏在集流体上施行可控原位组装低维碳材料的有效方法。针对该问题，本项目提出采用集流体衬底上构建的纳米结构模板结合所负载的过渡金属催化剂协同调控低维碳材料原位生长及组装的研究思路，系统考察碳纳米材料单元在纳米结构衬底构型和催化剂分布调控的协同影响下的组装行为和组装机理。项目主要研究内容可概述为：以碳布基底上生长的碳纳米线阵列作为纳米结构模板，控制碳纳米管活性材料的径向生长，获得具有高功率特性的超级电容器用电极；采用“自上而下”的化学刻蚀加工与赝电容电极材料的原位生长相结合的方法，实现金纳米沟槽衬底的制备和原位沉积痕量氧化锰电化学活性材料，获得了具有超高频率响应特性的电容储能性质；设计合成石墨烯和多孔碳纳米片结构保护模板，提高转化型负极材料的储锂、储钠性能。项目总结提出了低维碳纳米材料在纳米线结构衬底上组装构建超级电容器电极的新方法，并拓展研究了低维碳纳米材料作为结构保护模板提升锂、钠储能材料性能的有效途径，同时还提出新型纳米沟槽金属集流体的新加工方法。