金属氧化物/硫化物碳复合电极材料表面酸(碱)性与电化学性能的研究

The relationship of surface acid (alkali) center and the electrolytes ions was studied by the temperature programmed desorption (TPD) technology. We correlate this relationship, inherent structure, surface texture and electrochemical performance to reveal characteristic factors of the electrolyte transport speed during the charge and discharge progress and construct the practical theoretical control system of asymmetric supercapacitor or lithium battery electrode material structure and performance. In this work, the gelatin/GO/SiO2 composite precursor was prepared by self-assembly of gelatin and graphene oxide, and N, O-C/GO/SiO2 nanocomposites were prepared by nitrogen protection, in which the SiO2 sphere was prepared by Stöber methods. The SiO2 template was removed by HF etching while obtain 3D mesoporous N, O-C/GO carbon carriers. The sulfates or chlorides of Bi, Mo, W, Sn, Mn and V were used to prepare the composite of MxOy/MxSy @ 3D mesoporous N, O-C/GO electrode materials through of coprecipitate and hydrothermal methods. Hybrid supercapacitors, asymmetric supercapacitors and lithium-ion batteries were assembled in different organic electrolytes and ionic liquid electrolytes. The crystal structure, surface morphology and texture of MxOy/MxSy @ 3D mesoporous N, O-C/GO was studied. In addition, the surface heteroatom and regulation method of N, O-C/GO was also researched, which provide theoretical basis for exploitation of supercapacitor and battery electrode system materials with high voltage window, high energy density and high power density.

为了利用程序升温脱附技术，研究电极表面酸(碱)中心和电解质离子的作用关系，并与本证结构、表面织构和电化学性能相关联，揭示充放电过程中电解质离子的输运速度和传输的规律，建立混合型、非对称超级电容器或锂电池电极材料结构与性能调控的理论体系。本课题设计了Stöber法纳米SiO2球硬膜板和明胶和氧化石墨烯的水凝胶，经自组装-碳化-HF刻蚀脱硅制得N,O-C/GO3D介孔碳载体，然后，负载Bi、Mo、W、Sn、Mn和V的离子，经共沉淀和水热晶化合成制备MxOy或MxSy/N,O-C/GO三维孔结构复合电极材料。选用有机电解质和离子液体电解质，组装混合型、非对称型超级电容器或锂离子电池。详细研究MxOy或MxSy/N-C/GO复合电极的晶相结构、形貌以及空穴缺陷和表面织构以及掺杂原子基团的结构及其调控的有效途径，为高电压窗口、高能量密度和高功率密度的超级电容器及电池电极材料的研究与开发提供依据。

为满足碳中和和经济可持续发展，提高各类储能装置的充电/放电速率、功率密度和能量密度迫在眉睫，所以研究结构新颖的负极炭材料和金属化合物复合电极材料已成当务之急。针对蕴涵的科学问题，本课题着重开展了生物质基分级多孔炭材料和锂、钾离子电池正极材料体系的构建、合成制备、结构及其组装全电池的电化学储能机理的研究。优选软木、胶原蛋白、豆根、麻杆等生物质为碳源，基于上述思路，开展了① 高锰酸钾碳化氧化活化软木制备富氧分层级多孔炭及其电容性储能；② 碳酸钙活化法制备胶原蛋白基分级多孔炭及其CO2与H2的吸附性能；③ 铝掺杂介孔α-Ni(OH)2与豆根衍生炭非对称超级电容器储能性能；④ 高性能麻杆基强氧化剂活化多孔炭全固态对称超级电容器；⑤ 生物质衍生分级中孔碳超高效锂离子存储性能。基于高功率密度和高能量密度储能技术，进行了离子型混合超级电容器的研究，① 同源分层级多孔空心炭球负极与炭碗正极构建高性能钠离子混合超级电容器；② 分层级多孔中空炭球钾离子混合电容器的电化学性能及储能机理；③ 石墨烯网络葫芦脲[6]衍生氮掺杂分层多孔碳材料钾离子混合电容器；④ 葫芦脲[6]衍生亚纳米孔分层多孔碳材料混合超级电容器；⑤ 多维双碳骨架网络MnOx阳极高性能锂离子混合电容器；⑥ 超高掺硫分级多孔空心碳球负极的超级耐用钾离子混合电容器；⑦ 富氮磷共掺多孔碳电极高功率密度和高能量密度的钾离子混合电容器；⑧ 甘脲衍生多孔炭-石墨烯双炭网络负极材料钠离子混合电容器。开展了钾离子电池正极材料和镍钴过硒化物材料合成制备及结构的研究，① 离子交换法制备钾型水钠锰矿及其储钾、协同扩散、结构层间水与储钾性能；② 中空双晶相镍钴过硒化物制备与高性能混合超级电容器。总结分析高性能存储装置硅阳极：结构设计、材料复合、电解质和粘合剂的发展，构建研究了辅助导电缓冲结构的高性能锂离子电池硅阳极材料。还开展了基于炭基电光催化材料的研究，① [Zn4O(BDC)3]MOF-5修饰Ag3PO4光催化活性的研究；② 仿叶绿体基质结构Bi12TiO20/g-C3N4光催化性能降解有机污染物。本课题的研究结果为高性能储能装置的研发提供极具参考价值的理论依据。

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