In this study, we synthesized pH-controlled resorcinol-formaldehyde (RF) gels through the polymerization of two starting materials: resorcinol and formaldehyde. The prepared RF gels were dried using an acetone substitution method, and they were subsequently carbonized under nitrogen atmosphere to obtain carbon xerogels (CX_Y) prepared at different pH (Y). The carbon xerogels were utilized as active materials for coin-type organic supercapacitor electrodes to investigate the influence of pH on the electrochemical properties of the carbon xerogels. The carbon xerogels prepared at lower pH (CX_9.5 and CX_10) exhibited sufficient particle growth, with a three-dimensional network of particles during the RF gel formation, resulting in the development of abundant mesopores. Conversely, the carbon xerogels prepared at higher pH (CX_11 and CX_12) retained densely packed structures of small particles, leading to pore collapse and low specific surface areas. Consequently, CX_9.5 and CX_10 showed high specific surface areas, and provided ample adsorption sites for the formation of electric double layers with electrolyte ions. Moreover, the three-dimensional particle network in CX_9.5 and CX_10 significantly enhanced electrical conductivity. The presence of well-developed mesopores in these materials further facilitated the effective transport of electrolyte ions, contributing to their superior performance as organic supercapacitor electrodes. This study confirmed that pH-controlled carbon xerogels are one of the promising active materials for organic supercapacitor electrodes. Furthermore, we concluded that pH during RF gel formation is a crucial factor determining the electrode performance of the carbon xerogels, highlighting the need for precise pH control to obtain high-performance carbon xerogel electrodes.
Various carbon aerogels (CAs) were prepared from polymerization of resorcinol and formaldehyde and applied as the electrode materials of an electric double layer capacitor (EDLC) with the aim of controlling the textural and electrochemical properties of CAs by the type of base catalyst and the ratio of resorcinol to catalyst (R/C). The CAs from NaHCO3 and KHCO3 with H+ ions had higher specific surface areas but exhibited lower electrochemical properties than those from K2CO3 and Na2CO3, which had more uniform pore size distributions. The electrochemical properties of Na2CO3 were superior to those of K2CO3 probably because the polarizing power of Na+ ions was higher than K+ ions. With an increasing R/C ratio, the pore sizes of CA showed a tendency to increase but the uniformity of the pore size distribution got worse. For the four base catalysts, the highest electrochemical property was obtained at the R/C ratio of 500.
In this study, we intensively investigated the effect of conductive additive amount on electrochemical performance of organic supercapacitors. For this purpose, we assembled coin-type organic supercapacitor cells with a variation of conductive additive(carbon black) amount; carbon aerogel and polyvinylidene fluoride were employed as active material and binder, respectively. Carbon aerogel, which is a highly mesoporous and ultralight material, was prepared via pyrolysis of resorcinolformaldehyde gels synthesized from polycondensation of two starting materials using sodium carbonate as the base catalyst. Successful formation of carbon aerogel was well confirmed by Fourier-transform infrared spectroscopy and N2 adsorptiondesorption analysis. Electrochemical performances of the assembled organic supercapacitor cells were evaluated by cyclic voltammetry, galvanostatic charge/discharge, and electrochemical impedance spectroscopy measurements. Amount of conductive additive was found to strongly affect the charge transfer resistance of the supercapacitor electrodes, leading to a different optimal amount of conductive additive in organic supercapacitor electrodes depending on the applied charge-discharge rate. A high-rate charge-discharge process required a relatively high amount of conductive additive. Through this work, we came to conclude that determining the optimal amount of conductive additive in developing an efficient organic supercapacitor should include a significant consideration of supercapacitor end use, especially the rate employed for the charge-discharge process.
Activated carbons (ACs) have been used as EDLC (electric double-layer capacitor) electrode materials due to their high specific area, stability, and ecological advantages. In order to prepare ACs with high density and crystallinity, coal tar pitch (CTP) was activated by K2CO3 and the textural and electrochemical properties of the obtained ACs were investigated. Although the CTP ACs formed by K2CO3 activation had much smaller specific surface area and pore volume than did the CTP ACs formed by KOH activation, their volumetric specific capacitance (F/cc) levels as electrode materials for EDLC were comparable due to their higher density and micro-crystallinity. Structural characterization and EDLC-electrode performance were studied with different activation conditions of CTP/K2CO3 ratio, activation temperature, and activation period.
In order to prepare high-quality activated carbons (ACs), coal tar pitch (CTP), and mixtures of CTP and petroleum pitch (PP) were activated with KOH. The ACs prepared by activation of CTP in the range of 700~1000℃ for 1~5 h had very porous textures with large specific surface areas of 2470~3081 m2/g. The optimal activation conditions of CTP were determined as CTP/KOH ratio of 1:4, activation temperature of 900℃, and activation time of 3 h. The obtained AC showed the highest micro-pore volume, and pretty high specific surface area and meso-pore volume. The micro-pore volumes and specific areas of activated mixtures of CTP and PP were similar to each other but the meso-pore volume could be increased. In order to change the degree of crystallinity of precursors before KOH activation process, the CTPs were carbonized in the range of 500~900℃. As the carbonization temperature increased, the specific surface area and pore volume of the activated ACs with the same activation conditions for CTP decreased dramatically. It was demonstrated that the increased pore size distribution of AC electrodes in the range of 1 to 2 nm plays an important role in the performance of electric double-layer capacitor.
Commercial activated-carbon used as the electrode material of an electric double-layer capacitor (EDLC) was posttreated with various acids and alkalis to increase its capacitance. The carbon samples prepared were then heat-treated in order to control the amount of acidic functional groups formed by the acid treatments. Coin-type EDLC cells with two symmetric carbon electrodes were assembled using the prepared carbon materials and an organic electrolyte. The electrochemical performance of the EDLC was measured by galvanostatic charge-discharge, cyclic voltammetry, and electrochemical impedance spectroscopy. Among the various activated carbons, the carbon electrodes (CSsb800) prepared by the treatments of coconutshell-based carbon activated with NaOH and H3BO5, and then heat treated at 800˚C under a flow of nitrogen gas, showed relatively good electrochemical performance. Although the specific-surface-area of the carbon-electrode material (1,096m2/g) was less than that of pristine activated-carbon (1,122m2/g), the meso-pore volume increased after the combined chemical and heat treatments. The specific capacitance of the EDLC increased from 59.6 to 74.8 F/g (26%) after those post treatments. The equivalent series resistance of EDLC using CSsb800 as electrode was much lower than that of EDLC using pristine activated carbon. Therefore, CSsb800 exhibited superior electrochemical performance at high scan rates due to its low internal resistance.
Silicon-carbon composite was prepared by the magnesiothermic reduction of mesoporous silica and subsequent impregnation with a carbon precursor. This was applied for use as an anode material for high-performance lithium-ion batteries. Well-ordered mesoporous silica(SBA-15) was employed as a starting material for the mesoporous silicon, and sucrose was used as a carbon source. It was found that complete removal of by-products (Mg2Si and Mg2SiO4) formed by side reactions of silica and magnesium during the magnesiothermic reduction, was a crucial factor for successful formation of mesoporous silicon. Successful formation of the silicon-carbon composite was well confirmed by appropriate characterization tools (e.g., N2 adsorption-desorption, small-angle X-ray scattering, X-ray diffraction, and thermogravimetric analyses). A lithium-ion battery was fabricated using the prepared silicon-carbon composite as the anode, and lithium foil as the counter-electrode. Electrochemical analysis revealed that the silicon-carbon composite showed better cycling stability than graphite, when used as the anode in the lithium-ion battery. This improvement could be due to the fact that carbon efficiently suppressed the change in volume of the silicon material caused by the charge-discharge cycle. This indicates that silicon-carbon composite, prepared via the magnesiothermic reduction and impregnation methods, could be an efficient anode material for lithium ion batteries.