Functional Carbonaceous Networks as Electrodes in Energy Storage Devices

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The advancement of electrochemical energy storage systems highly depends on the development of novel high performance electrode materials. While a variety of inorganic and organic electroactive materials have been investigated, heteroatom-doped and/or functionalized carbon materials have recently attracted much attention because of their great potential in high performance electrochemical energy storage devices including lithium ion batteries and electrochemical capacitors. Yet, in most cases reported previously, the concentration, distribution, and bonding state of heteroatoms and/or oxygen-containing functional groups in the parent carbon structures (e.g., carbon nanotubes or graphene) are hardly controllable based on the existing synthetic techniques, which significantly limits the evaluation of the influence of heteroatoms doped into carbon materials on their electrochemical performance. Conjugated highly cross-linked porous polymer networks on the other hand enable a highly defined incorporation of functional groups or heteroatoms. However, their usage for electrodes is rather limited as these networks display low conductivities. In this project we will prepare functional carbonaceous networks by rational synthesis and controlled pyrolysis of conjugated polymer networks with specific functionalities, as well as construct their composites with other electrically conductive materials such as carbon nanotubes, graphene, and nanoscale metallic current collectors. These novel materials and composites will be exploited as electrodes in energy storage devices, with emphasis on the understanding of the structure-property relationship of these carbon-based electrodes. Combined with a comprehensive investigation of the effect of chemical functionalities, structure, and interfaces of functional carbonaceous networks and their composites on their electrochemical performance, the project will provide a new class of high performance asymmetric electrochemical cells using optimized functional carbonaceous network-based electrodes.