CNT纤维的可控电化学功能化：结构-化学关系及其在无集流体全固态超级电容器中的应用
Controlled electrochemical functionalization of CNT fibers: structure-chemistry relations and application in current collector-free all-solid supercapacitors
摘要：
纳米碳的化学官能化是通过产生具有额外法拉第贡献的表面官能团、通过增加它们的表面积和相应的电容贡献以及通过改善与水性电解质和其它活性材料（例如赝电容金属氧化物）的相容性来产生具有更高能量/功率密度的电化学系统的重要策略。在这里，我们提出了一种电化学方法，同时溶胀和功能化的碳纳米管，使材料亲水性的宏观纤维织物组成的大电极，并产生比电容和能量密度在水性电解质的大幅增加。通过拉曼光谱、透射电子显微镜、X射线光电子能谱（XPS）和小角X射线散射（SAXS）对碳纳米管纤维（CNTF）进行深入表征，我们确定了对这种改进的各种贡献，包括表面氧化、管状解链、解束和束间溶胀。通过分析极性和非极性液体在电极中的扩散动力学，确定功能化CNTF的亲水性变化。提取的接触角和极性和色散的表面能成分为不同的处理条件下是一致的偶极距的变化通过XPS获得。最后，功能化CNTF电极中采用的电流收集器自由固体柔性超级电容器，这表明增强的电化学性能相比，所产生的疏水性。
英文摘要：
Chemical functionalization of nanocarbons is an important strategy to produce electrochemical systems with higher energy/power density by generating surface functional groups with additional faradaic contribution, by increasing their surface area and correspondent capacitive contribution and by improving compatibility with aqueous electrolytes and other active materials, such as pseudocapacitive metal-oxides. Here we present an electrochemical method to simultaneously swell and functionalize large electrodes consisting of fabrics of macroscopic fibers of carbon nanotubes that renders the material hydrophilic and produces a substantial increase of specific capacitance and energy density in aqueous electrolytes. Through in-depth characterization of the carbon nanotube fibres (CNTF) by Raman spectroscopy, transmission electron microscopy, X-ray photoelectrocn spectroscopy (XPS) and small-angle X-ray scattering (SAXS) we identify various contributions to such improvements, including surface oxidation, tubular unzipping, debundling and inter-bundle swelling. Changes in hydrophilicity of functionalized CNTF are determined by analyzing the dynamics of spreading of polar and nonpolar liquids in the electrode. The extracted contact angles and polar and dispersive surface energy components for different treatment conditions are in agreement with changes in dipole-moment obtained by XPS. Finally, functionalized CNTF electrodes were employed in current collector-free solid flexible supercapacitors, which show enhanced electrochemical properties compared to as-produced hydrophobic ones.
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