活化石墨烯薄膜层间“柱撑”式规整离子通道的构筑及储能研究

The development of advanced electrodes with high density and high ions transfer rate is essential for the next-generation high-rate energy storage devises. The graphene film self-assemble progress has a poor control over the nanostructure, the disordered distribution and shrinking of graphene flakes results high ions transfer resistance, thus influence the electrode rate performance. Herein, this project expect to fabricate a densely packed activation graphene film with highly ordered graphene flakes distribution and efficient interlayer ions transfer pathways by combination the internal/external force field and chemical activation. The controllability of the graphene film regularity and interlayer uniformity will discussed by study the coupling influence of the internal/external force field during film fabrication; the confined porous nano-structure formed inside the graphene film interlayer will adjusted by the activation process and control over the pillar structure; the flexibility and mechanical stability of the active graphene film will discussed by measuring the nano-structure of the film; the ion diffusion rate inside the activated graphene film as well as its relationship with the porous nano-structure of the membrane will also studied. This research will pave a way for the advanced high density, high rate graphene-based energy storage electrodes.

高密度、高离子迁移效率新型电极的制备对开发高倍率储能器件具有重要意义。当前石墨烯薄膜自组装过程层间微纳结构可控性差，片层不规则分布及折叠褶皱造成层间离子迁移阻力大，影响电极倍率性能。基于此，本项目提出利用内外力场耦合制备片层规整排布、利用化学活化构筑层间支撑及高效离子迁移通道的致密薄膜电极制备思路。通过研究成膜过程内外力场对石墨烯片层规则化排布的耦合作用机制，阐明石墨烯薄膜片层规整度及层间距均匀性的调控规律；通过探索薄膜化学活化过程层间“柱撑”结构及离子迁移通道的构筑机理，明确活化异构对石墨烯薄膜密度及限域微纳结构的调控机制；通过考察活化石墨烯压力/折叠条件下层间微纳结构变化规律，探明活化异构对薄膜机械性能的提升机制；通过研究活化石墨烯薄膜层间限域微纳结构与离子迁移效率的构效关系，探明层状薄膜材料层间离子迁移强化机制。研究结果将为设计和制备高密度、高倍率新型石墨烯薄膜电极奠定理论基础。

高密度、高离子迁移效率新型电极的设计制备对开发高倍率储能器件具有重要意义。通过调控石墨烯基复合薄膜纳米片层取向及平整结构，构造规整的电解液层间限域传质通道，同时实现电子的高效传输，是设计制备高密度碳基电极材料的关键。基于此，本项目主要针对石墨烯基复合电极片层规整化取向及均匀层间柱撑结构调控展开研究，研究了内外力场协同取向平整片层结构、插层柱撑规整结构与层间距调控、规整层间结构传质效率强化及结构稳定机制、规整层间结构与储能性能构效关系等方面的基础科学问题，深入探讨了高密度石墨烯复合薄膜电极的设计构筑及性能强化机制，并进一步探讨了高传质效率碳基复合电极的设计制备。取得的研究成果如下：1、设计了内外力场协同的石墨烯薄膜片层规整化取向及高效传质通道构筑方案，利用纳米片、阳离子实现了层间插层柱撑结构的精细调控，实现了石墨烯片层的高度平整取向及规整层间结构的构筑，探讨了规整结构对层间传质效率与储能性能的强化机制；2、探讨了低成本梯度孔结构多孔碳微纳结构设计制备及传质过程强化机制，实现了具有梯度多孔结构碳材料的高效制备及传质效率的强化；3、实现了平行翅片取向纳米晶结构可控构筑及准二维限域通道的传质强化，通过电极微纳结构的理性设计实现了传质性能与电化学性能的双效提升；4、研究了碳基多层级导电网络微纳结构理性设计及导电/传质过程强化，探讨了多级导电网络设计对电子/离子迁移效率、活性物质可控负载及电化学性能的协同强化规律。相关结果在以第一作者或通讯作者在SCI杂志发表高水平论文26篇。