基于电化学技术快速可控制备石墨烯及其应用性能

As one of carbon family members, graphene has been known as a sharply rising star after the discovery of fullerene and carbon nanotubes, and has drawn much attention due to its wide application potential in a number of fields. However, how to produce graphene with tuned structure and properties cheaply and quickly remains a big challenge. In this proposal, coal, a kind of cheap and abundant carbon source, will be used as the carbon source to prepare graphene. For this purpose, the electrochemical approach under the drive of direct/alternate current will be adopted, with an aim of tuning the size and chemical properties of the graphite crystallites resulting from the coal, further producing the graphene that is excellently conductive, controllable defective density, and more easily processible. The relationship between the structure and properties of the starting coal and the as-made graphene will be explored, which will help to optimize the electrochemical processes that will be capable of tuning the properties, microstructures of the carbon sources and the as-made graphene. The dependence of the conductivity, defective density and the solution-processible behavior of the as-made graphene on the size, shape, surface chemistry, dispersing properties and the microstructure will be examined, which will reveal the mechanism governing the conductive and solution-processible properties of the graphene. With the help of quartz crystal microbalance, the principle for electrochemical exfoliation will be detected, unveiling the intercalation, oxidation/reduction process. The potential of the as-made graphene and graphene-based composites as electrode in supercapacitor device will be explored. The corresponding mechanism for electronic transfer and charge storage will be decoupled. This project will help shed a new light on the low cost production of high quality graphene derived from coal and their structure-properties relationship, which will surely help to further improve the understanding of the carbon science and technology in general and the coal-based functional carbon nanomaterials in particular.

结构和性能可调变石墨烯的廉价快速可控制备及其性能的精准调变是一个富有挑战性的课题。本项目提出以煤为碳源，采用直流/交流电场辅助技术策略，基于对煤炭中石墨微晶的调控策略，快速可控制备具有优异导电性和可加工性的煤基石墨烯。研究揭示石墨烯的结构与碳源的结构和化学性质及预处理工艺条件间的规律关系；研究不同电场作用下煤基石墨形成的机理和差异，及电解液离子的迁移行为；建立结构和性能可控的煤基石墨烯之制备技术策略。辅以石英微晶天平和原位拉曼技术，解耦煤基石墨烯形成过程中氧化/还原行为的差异及其生成机制。揭示煤基石墨烯的电子传输和储能机制与其尺寸、分散性、微观结构等之间的构效关系，及石墨烯电子输运效应的本质；探究煤基石墨烯及其复合新结构杂化材料在超级电容器领域的应用潜力和特点。项目的实施将为高性能煤基炭素材料及其复合材料的低成本创制奠定坚实的科学基础，成果将丰富和发展碳材料学科的内涵，有重要学术价值。

结构和性能可调变石墨烯的廉价快速可控制备及其性能的精准调变是一个富有挑战性的课题。项目研究提出了基于电化学技术快速可控制备石墨烯及其复合材料的策略，实现了石墨烯结构、组成、表面物理和化学性质的调控。揭示了影响石墨烯结构、组成、缺陷密度、物理和化学性质和性能的关键因素，并建立了相应的调控技术策略。揭示了电化学技术制备石墨烯插层氧化/还原机制。研究了石墨烯及其功能化技术并探索其应用领域探索和应用之研究。建立了石墨烯物理和化学原位修饰与功能化的技术方法。研究了石墨烯及其复合材料在超级电容器、电催化等领域的应用潜力。上述工作丰富和发展了碳材料学科的内涵，有重要学术价值和潜在的应用前景。围绕上述工作，项目执行期间，作为项目负责人，获批1项国家自然科学基金面上项目，获批1项大连市杰青项目，获批1项中央高校基本科研业务费项目；作为骨干，参加科技部国家重点研发计划重大项目3项。围绕上述工作，近4年，在材料化工领域主流国际学术刊物ACS Nano、Nature Communication等接收/发表SCI论文30余篇（已标注资助21篇）。申请/授权专利10件。项目负责人担任J Energy Chem的Section Editor（执行编委）、Chin Chem Lett高级编委、《煤炭转化》编委等刊物编委。。.指导培养的研究生，多人次获得国家和省部级的奖励。1名获2022年度化学化工与材料京博优秀博士论文奖(优秀奖)，1名获2021年度化学化工与材料京博优秀博士论文奖(提名奖)，1名博士生获辽宁省优秀毕业生，1名获2020年度辽宁省优秀博士论文奖，1名获2019年度辽宁省优秀博士论文奖(提名奖)等。.项目负责人2021年受聘教育部长江学者特聘教授，荣获2019“侯德榜化工科学技术青年奖”、2019大连市高层次人才创新支持计划--大连市杰出青年科技人才等荣誉和表彰。入选英国皇家化学会2019 Top1%高被引中国作者、科睿唯安2022年度“高被引科学家”名单。作为主要完成人之一，获2019年辽宁省自然科学一等奖、2020中国颗粒学会自然科学一等奖。