碳基超级电容器具有充放电时间短、使用温度范围宽、循环寿命长、安全性能好等诸多优点，是最具应用前景的新型储能装置之一。但是，与二次电池相比，其能量密度较低。在保持碳基超级电容器高比功率的前提下，通过调控多孔碳电极材料的孔隙结构来提高其能量密度是该领域的研究重点。研究表明，孔径与净电解液离子尺寸相当的超微孔碳拥有大比容量储能特性，但介/大孔尺度的离子传输通道的缺乏影响其大倍率充放电性能。本文提出以具有分子内有机/无机杂化特点的多面体低聚倍半硅氧烷（POSS）作为碳源和产生均匀微孔的自模板，嵌段共聚物聚集体或者胶态晶体为产生有序介孔的软、硬模板，合成出有序微/介分级孔碳。具体内容如下：

       1. 提出一种基于POSS与两亲性Pluronic型三嵌段共聚物PEO-PPO-PEO间自组装合成分级多孔碳的新方法。由于POSS分子中硅氧笼的分子尺度模板效应以及嵌段共聚物和所用的胺基功能化POSS化合物（笼型八胺苯基倍半硅氧烷，OAPS）间良好的组装适应性，所得碳既拥有十分均匀的微孔（尺寸~1 nm），也拥有高度有序的介孔（尺寸~4 nm），同时，还具有超过2000 m² g⁻¹的高比表面积和超过1.19 cm³ g⁻¹的大孔容。通过简单地采用具有不同PEO/PPO比的嵌段共聚物，材料的介观对称性可以为二维六方（p6m）和体心立方（）。另外，因为OAPS为富含氮元素的碳源前驱体，氮官能团也能自发掺杂到碳材料中。由于该类分级孔碳具有孔径接近电解液离子尺寸的均匀微孔，其在净离子液体电解液中最大比容量达~163 F g⁻¹，在1.0 M H₂SO₄水系电解液中达~216 F g⁻¹。由于能够显著减小电荷传递阻力，该类分级孔碳与纯微孔碳相比表现出良好的倍率性能。当电流密度从0.25增至10 A g⁻¹，最优试样在净离子液体和1.0 M H₂SO₄电解液中容量保持率分别可达94%和97%。

       2. 由于商品化的Pluronic型三嵌段共聚物种类相对有限且分子量较低（通常M_w < 15000），由其胶束模板产生的有序介孔尺寸一般难以超过5 nm。为了研究介孔孔径对分级孔碳电容性能的影响，我们进一步以氧化硅胶态晶体为模板，笼型八胺苯基倍半硅氧烷（OAPS）为碳源，制备出含三维有序介孔、介孔孔径在14~40 nm范围内精确可调的有序微/介分级孔碳。结果表明，在净离子液体电解液中，随着介孔孔径增加，所得分级孔碳的倍率性能呈下降趋势。这可能是因为介孔孔径的增大也伴随着孔壁的明显变厚，反而增大了电解液向孔壁微孔内迁移、扩散的阻力。具有最小介孔孔径（~14 nm）的碳试样在电流密度为0.25 A g⁻¹时比容量达172 F g⁻¹，在电流密度增大至20 A g⁻¹时仍有148 F g⁻¹，容量保持率为86%，表现出良好的倍率性能。

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