近年来,用于电化学能源存储和转化的石墨烯材料,得到了研究者们越来越多的关注。但是,这些石墨烯材料不同于严格定义的单原子碳层结构,往往具有孔洞、杂原子和化学官能团等缺陷结构。由于制备方法的不同,缺陷结构各不相同,其电化学性能也表现各异。结构分析表明,这类材料是由类似石墨烯片段的单元与聚合物链共价连接而成,使其具有石墨烯和聚合物的双重特性,我们称之为石墨烯化聚合物。由小分子通过自下而上的方法制备的多孔聚合物,也可以通过进一步热交联等方法,使其形成包含石墨烯片段单元与聚合物链的化学结构。这些材料与石墨烯衍生材料一起组成了石墨烯化聚合物的整个谱系;这个谱系涵盖了由聚合物到石墨烯的过渡区。更重要的是,这类材料特殊的结构与性质,使其成为一种兼具电子和离子传输通道的三维富碳高分子材料,非常适合作为电极材料应用于电化学能源存储和转化,这为我们深入研究储能器件中电极材料的结构与性能的相关关系提供了很好的材料平台。
Graphene and its derivatives have attracted increasing attention during the last decade as efficient materials for the storage and conversion of energy. In most cases, however, these graphene materials possess large numbers of structural defects such as cavities, heteroatoms and functional groups, making them quite different from the precisely-defined "single carbon layer of graphite" observed for graphene. These materials also differ considerably in terms of their electrochemical properties because of their variable structures, which are strongly influenced by the methods used during their preparation. Structural analyses have indicated that these materials consist of graphene subunits, which are interconnected by organic linkers with properties lying between those of graphene and polymers, which we have defined as "graphenal polymers". The thermal crosslinking reactions of porous polymer networks fabricated from small organic molecules using a bottom-up strategy also result in graphene-like subunits, which are covalently interconnected by polymeric fractions. These materials cover a series of transitional intermediates belonging to the "graphenal polymers" family, where polymers and graphene sit at opposite ends of family spectrum. Moreover, the special structures and properties of these materials make them ideal electrode materials for the storage and conversion of energy via electronic and ionic transport pathways, allowing for a deeper evaluation of the structure-property relationships of different electrode materials.