基于金属纳米网集流体的透明柔性石墨烯基多级结构电极的双电层电容性能研究

Aiming to research on the structures and performances of the electrode materials for novel transparent, flexible supercapacitors, this proposed project is based upon the strategy in introduction of metal nano network transparent, flexible electrodes as current collectors and graphene nanosheets coupled with various carbonaceous materials deposited corresponding to the relative position of the metal nano network as hierarchically structured electrodes for supercapacitors, which could be fabricated by means of spin-coating and electrodeposition, respectively. The microstructures and the transparency of the metal nano network and the electrode materials could be tailored by control of the size of the raw materials and the synthesis parameters, and analyzed by various materials characterization techniques. Meanwhile, the double-layer capacitive performance of the electrode could be systematically evaluated by means of cyclic voltammetry (CV), galvanostatic charge/discharge and electrical impedance spectroscopy (EIS) through electrochemical workstation. The mathematic model of the relationship of the component, thickness, mass loading density and conductivity with regard to the transparency and double-layer capacitive performance of the electrode materials will be established. The interaction effects of the graphene based hierarchically structured electrodes with regard to the transparency and double-layer capacitive performance of the supercapacitor will be revealed. The intrinsic nature of the charge storage, transportation and diffusion in the novel system of the transparent, flexible supercapacitor based upon the metal nano network, graphene nanosheets and carbonaceous material components will also be illustrated. The implementation of this proposed project will be expected to provide prototypes and experimental, theoretical supports towards the development of the novel transparent, flexible supercapacitor, which matters significantly and possesses comprehensive application prospect.

为了研究新型透明柔性超级电容器电极材料结构和性能，本申请拟利用旋涂法制备金属纳米网透明电极作为集流体，结合电沉积技术制备与金属纳米网集流体相对应的石墨烯基多种炭材料相结合的多级结构电极材料，通过控制原料尺度、调整制备技术参数结合材料表征技术对金属纳米线、电极材料的微观结构以及极片的透光率进行全面分析。同时通过电化学工作站利用循环伏安法、恒电流充放电和交流阻抗谱对极片的双电层电容性能进行全面测试，构建电极材料组分、厚度、极片覆料密度、电导率与超级电容器的透光率以及双电层电容性能指标的数学模型，揭示石墨烯基电极的多级结构与透光率、双电层电容性能之间相互影响规律，阐明石墨烯纳米片、其他炭材料组分、金属纳米线在透明柔性超级电容器新体系中的电荷存储、输运和扩散的物理本质。该申请项目完成后所取得的成果可望为开发新型透明柔性超级电容器提供新的技术原型和数据、理论支持，具有重要的理论意义和广阔的应用前景。

透明柔性超级电容器是未来消费电子产品中重要的集成电源之一，它的设计和研发对于实现全透明柔性电子产品起到至关重要的推动作用。本项目设计了以电泳沉积技术制备的石墨烯@银纳米线/PET透明电极，石墨烯为活性材料层，制备了基于双电层机制的三明治夹层结构透明柔性超级电容器。一方面，柔性石墨烯层可以防止银纳米线在电解质环境中被氧化；另一方面，具有褶皱形貌且贴合紧密的石墨烯层可以存储电荷，并且石墨烯层和银纳米线可以构成共渗透的传导网络结构，有效地传输电子，彼此间的协同作用赋予了透明柔性超级电容器优异的性能。通过加入碳纳米管，增加相邻石墨烯层的层间距，进而可提供一个开放的三维结构便于电荷的存储和传输。与此同时，引入的纳米碳管可以促进石墨烯层间的电子传输，提高垂直于石墨烯层方向的电子导电率。碳纳米管支撑的石墨烯层与银纳米线网络相结合也形成了共渗透薄膜结构，从而使得制备的透明柔性超级电容器在保持高透光率前提下还兼备了优良的电荷存储能力、机械稳定性。通过对石墨烯活性层的真空冷冻干燥处理，有效的保持了石墨烯层状结构，更重要的是使石墨烯膜层间距加大，石墨烯片层褶皱化程度加大，比表面积增加，石墨烯活性层/电解质界面的电荷储存能力显著提升。另外，通过界面电容概念的引入探讨了石墨烯层间结构与测量的面积比电容之间的关系，加深了对透明柔性超级电容器中石墨烯活性层双电层电荷存储能力本质的理解。本项目的研究揭示了新体系中石墨烯基活性材料层与银纳米网的电荷存储、输运和扩散的物理本质，为开发新型透明柔性超级电容器提供新的技术原型和数据、理论支持。.在本项目执行期间，以第一作者或通讯作者共发表SCI论文10篇，包括Advanced Functional Materials, Journal of Materials Chemistry A, Nano Energy等，其中影响因子大于10的2篇，JCR一区论文9篇。上述论文全部标注基金资助号51502073。共参加学术会议4次，口头报告1次。申请发明专利5项，其中授权2项。协助培养毕业硕士研究生2名，在读研究生2名，本科生2名。

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