壳聚糖基含N碳气凝胶的制备、结构与性能调控

N-rich carbon materials show their great potentials in water treatment, CO2 adsorption, battery, supercapacitor, and catalysis due to their outstanding adsorption, conductivity, electrochemistry, and catalysis properties. Fabrication of sustainable, cost-efficient and high-quality N-rich carbon materials by using low-cost, renewable, environment-friendly, and abundant chitosan as C and N sources is an ideal rout to substitute petroleum-based N-rich carbon materials. In this study, with the arm to solve the structure and property regulations of chitosan-based N-rich carbon material, N-rich carbon aerogel with hierarchical structure will be fabricated by using chitosan aerogel as a controllable precursor. The influences of the porous structure of precursor, carbonization, catalysis, and activation on the physicochemical characteristics and supercapacitor property of the N-rich carbon aerogel are to be investigated. The N fixation behavior and regulation of N-rich carbon aerogel during carbonization, as well as related mechanisms, will be also studied to allow a better comprehension of the structure and property controls of N-rich carbon aerogel and obtain novel carbon materials with high-quality supercapacitor property. This study will greatly help to address the structure and property regulations of chitosan-based N-rich carbon material, and obtain N-rich carbon aerogel with excellent supercapacitor property. This study will also provide effective routs for fabrication of high-quality biomass-based N-rich carbon materials and their applications.

含N碳材料具有更优异的吸附性能、导电性、电化学性能、催化性能等，在水处理、CO2吸附、电池与超级电容器、催化等领域具有巨大的应用前景。以廉价、可再生、环境友好、丰富的生物质壳聚糖为C源和N源合成低成本、高性能含N碳材料是替代石化基含N碳材料的理想途径，是可持续的新型碳材料。本项目针对目前壳聚糖基含N碳材料结构与性能调控问题，提出以壳聚糖气凝胶为前驱体合成具有分级孔隙结构的含N碳气凝胶，从壳聚糖气凝胶的微观孔隙结构、碳化条件、催化、活化处理等方面深入研究此类含N碳气凝胶理化结构与超级电容性能的影响与调控途径，并对碳化过程N固留行为和调控途径进行探讨，阐明相关规律与机制。项目的开展及预期成果的获得不仅可解决壳聚糖基含N碳气凝胶结构调控与性能提高问题，获得高性能新型含N碳材料，而且为可持续发展的生物质基高性能含N碳材料的合成、应用提供新思路与有效途径。

本项目以生物质N源为前驱体，采用溶解-凝胶、冷冻干燥、模板法等方法制备合成了具有分级孔隙结构的碳气凝胶，从碳气凝胶的微观孔隙结构、碳化条件、催化、活化等方面系统研究了此类碳气凝胶理化结构与超级电容性能、机械性能、传感性能的影响与调控途径，并阐明相关规律与机制。进一步以制备的碳气凝胶为多孔载体、结构单元构建了高性能的复合电极材料与柔性电极材料。制备的碳气凝胶的比电容高达373 F g-1，能量密度达22.2 Wh kg-1，且具有良好的循环稳定性。制备的可压缩弹性碳气凝胶具有高压缩性（95%）、超弹性，稳定的应变电流响应和抗疲劳性。尤其是，材料具有超高灵敏度，达103.5 kPa-1，且0-18 kPa范围保持良好的宽线性灵敏度，实现了在宽压力范围对压力的准确检测。研究成果发表SCI研究论文10篇，其中影响因子高于5.0 的论文7篇，最高影响因子21.950；申请国家专利4 件。研究成果为碳气凝胶的制备与应用提供了有效新技术与新理论，得到国内外同行的高度评价，SCI它引150多次，1篇论文入选高被引论文。