石墨烯基高比能超级电容器关键材料与器件性能研究

Taking into the full considerations of the current status of graphene materials and urgent demands of supercapacitors with high specific energy, high power density, flexibility and miniaturization, this project aims at the key scientific problems of graphene-based high-energy supercapacitors, including the innovative preparation of key materials, device assembly, in-situ characterization, theoretical calculation and other important aspects of electrolytes and current collectors. To this end, the major science & technology objectives include the following aspects: (i) to innovatively prepare high-quality graphene based materials, such as activated graphene, graphene-like porous carbon in a large scale, to assembly different dimensional graphene macroscopic monoliths of such as fibers and films, and to construct compact graphene hybrid electrode materials of such as graphene/Li4Ti5O12 with high specific capacitance; (ii) to design and screen high voltage and stable electrolytes, such as water-in-salt electrolyte, redox electrolyte, ionic electrolyte, gel electrolyte, for the designable supercapacitors; (iii) to create high-energy and new-concept supercapacitors, including lithium ion batteries, ionic liquid supercapacitors, flexible and micro-supercapacitors, using advanced technology of device assembly, (iv) to illustrate the charge-storage mechanism of the resultant devices with the combined in-situ characterization study and theoretical simulation means. Through the successful implementation of this project, the key materials and advanced device technologies, with independent intellectual property rights and international core competitiveness, are obtained to provide the technical and scientific guidance for the future development of supercapacitor industrialization.

本项目将结合石墨烯材料和超级电容器产业的发展现状，以高比能、柔性化、集成化等军民两用超级电容器的需求为牵引，聚焦石墨烯材料在储能领域中亟待解决的关键科学问题，将在超级电容器关键材料制备、器件组装、原位表征、理论计算等方面进行协同创新。以构筑高比容量石墨烯电极材料为研究对象，建立石墨烯、高比表面积石墨烯活性炭、寡层石墨烯类孔碳等高容量电极材料制备新技术，发展规模化技术生产钛酸锂/石墨烯等关键电极材料；以高电压质子型电解液、混合型电解液、离子液体为新型电解液，设计并优化高性能、柔性化、集成化超级电容器的组装工艺，研发出高比能石墨烯超级电容器，发展高比能储能单体等关键电极材料与器件技术。结合原位表征测试系统和理论模拟，揭示石墨烯基超级电容器储能机理，建立电化学存储理论模型，为发展石墨烯关键电极材料和构筑高比能超级电容器提供科学指导。

本项目针对我国石墨烯材料和超级电容器产业的发展现状，以高比能、柔性化、集成化等军民两用超级电容器的需求为牵引，主要围绕高容量石墨烯基关键电极材料的开发，高比能锂离子超级电容器构筑与机理研究，以及高比能、柔性化超级电容器构筑与系统集成三个方面开展了系统性工作，取得了一系列的成果：（i）发展了电化学剥离法、KOH活化法、液氮冷萃法、激光热解法、自蔓延燃烧法、界面自组装法、软/硬模板法、石墨烯二维模板法等新策略，制备出多种高比表面积、高导电性、孔隙发达的石墨烯基高比能超级电容器关键电极材料；（ii）开发出多种高性能锂离子超级电容器正负极材料，提出了容量和动力学双匹配策略，构筑出高性能双电层电容器、多电子赝电容期以及电池型锂离子电容器；（iii）提出了光刻、掩膜版辅助过滤、激光热解、丝网印刷、喷墨打印、3D打印等高精度、规模化微加工技术，发展了多界面协同调控策略，研制出多种石墨烯基柔性化、微型化超级电容器及其微能源系统，揭示了离子多方向传输机制。.在项目执行期间，申请人在Energy Environ. Sci.（4篇）、Adv. Mater.（3篇）、Adv. Energy Mater.（4篇）、Nature Commun.、Angew. Chem. Int. Ed（2篇）、Adv. Funct. Mater.（5篇）、Adv. Sci.、Energy Storage Mater.（7篇）、Natl. Sci. Rev.等国际权威杂志发表论文79篇，其中IF>10的论文65篇；申请发明专利35项，已授权的2项；应邀在国际国内重要会议做大会报告和邀请报告60余次。申请人获得国家杰出青年科学基金获得者、第十三届辽宁青年科技奖、英国皇家化学会会士、2019-2022年科睿唯安全球高被引科学家、爱思唯尔中国高被引学者、中国科学院优秀导师奖等奖励/荣誉。担任Applied Surface Science副主编、J. Energy Chem.执行编委，Energy Storage Mater.、Natl Sci. Rev.、Sci. Bull.、eScience等期刊编委。担任超级电容产业联盟青年工作委员会副主任。该项目的顺利实施为合理设计石墨烯基高比能超级电容器关键材料和构筑高性能锂离子超级电容器、柔性化微型超级电容器及集成系统提供重要的科学基础。