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.

본 연구는 에너지 저장 응용을 위한 PVI-PGMA/LiTFSI 고분자 막 전해질 및 CxNy-C 유연 전극의 합성 및 특성 에 관한 연구이다. 이중 기능을 갖는 PVI-PGMA 공중합체는 우수한 이온 전도성을 나타내었으며, PVI-GMA73/LiTFSI200 막 전해질은 1.0 × 10-3 S cm-1의 최고 전도도를 달성하였다. CxNy-C 전극의 전기화학적 성능을 체계적으로 분석하였으며, C3N2-C는 나노와이어와 다면체로 구성된 높은 연결성을 갖는 하이브리드 구조와 이중 Co/Ni 산화물을 포함하여 풍부한 산 화환원 활성 부위와 이온 확산을 용이하게 하는 특징으로 인해 958 F g-1의 최고용량 및 최소한의 전하 전달 저항(Rct)을 달성 하였다. 흑연 탄소 껍질의 존재는 충전-방전 동안 높은 전기화학적 안정성에 기여하였다. 이러한 결과들은 고성능 에너지 저 장 장치인 슈퍼커패시터 및 리튬 이온 전지와 같은 첨단 에너지 저장 장비에 PVI-PGMA/LiTFSI 고분자 막 전해질과 CxNy-C 전극을 활용하는 잠재력을 보여주었으며, 지속 가능하고 고성능의 에너지 저장 기술을 더욱 발전시키는 길을 열어가 고 있다.

The recycling of solid waste materials to fabricate carbon-based electrode materials is of great interest for low-cost green supercapacitors. In this study, porous carbon foam (PCF) was prepared from waste floral foam (WFF) as an electrode material for supercapacitors. WFF was directly carbonized at various temperatures of 600, 800, and 1,000 oC under an inert atmosphere. The WFF-derived PCF (C-WFF) was found to have a specific surface area of 458.99 m2/g with multi-modal pore structures. The supercapacitive behavior of the prepared C-WFF was evaluated using a three-electrode system in a 6 M KOH aqueous electrolyte. As a result, the prepared C-WFF as an active material showed a high specific capacitance of 206 F/g at 1 A/g, a rate capability of 36.4 % at 20 A/g, a specific power density of 2,500 W/kg at an energy density of 2.68 Wh/kg, and a cycle stability of 99.96 % at 20 A/g after 10,000 cycles. These results indicate that the C-WFF prepared from WFF could be a promising candidate as an electrode material for high-performance green supercapacitors.

Fibrous supercapacitors (FSs), owing to their high power density, good safety characteristic, and high flexibility, have recently been in the spotlight as energy storage devices for wearable electronics. However, despite these advantages, FCs face many challenges related to their active material of carbon fiber (CF). CF has low surface area and poor wettability between electrode and electrolyte, which result in low capacitance and poor long-term stability at high current densities. To overcome these limits, fibrous supercapacitors made using surface-activated CF (FS-SACF) are here suggested; these materials have improved specific surface area and better wettability, obtained by introducing porous structure and oxygen-containing functional groups on the CF surface, respectively, through surface engineering. The FS-SACF shows an improved ion diffusion coefficient and better electrochemical performance, including high specific capacity of 223.6 mF cm2 at current density of 10 μA cm2, high-rate performance of 171.2 mF cm2 at current density of 50.0 μA cm2, and remarkable, ultrafast cycling stability (96.2 % after 1,000 cycles at current density of 250.0 μA cm2). The excellent electrochemical performance is definitely due to the effects of surface functionalization on CF, leading to improved specific surface area and superior ion diffusion capability.

높은 안전성과 견고한 기계적 특성을 가진 고체상 슈퍼커패시터는 차세대 에너지 저장 장치로서 세계적 관심을 끌고 있다. 슈퍼커패시터의 전극으로서 경제적인 탄소 기반 전극이 많이 사용되는데 수계 전해질을 도입하는 경우 소수성 표 면을 가진 탄소 기반 전극과의 계면 상호성이 좋지 않아 저항이 증가한다. 이와 관련하여 본 연구에서는 전극 표면에 산소 플라즈마 처리를 하여 친수화된 전극과 수계 전해질 사이의 향상된 계면 성질을 기반으로 더 높은 전기화학적 성능을 얻는 방법을 제시한다. 풍부해진 산소 작용기들로 인한 표면 친수화 효과는 접촉각 측정을 통해 확인하였으며, 전력과 지속시간을 조절함으로써 친수화 정도를 손쉽게 조절할 수 있음을 확인하였다. 수계 전해질로 PVA/H3PO4 고체상 고분자 전해질막을 사 용하였으며 프레싱하여 전극에 도입하였다. 15 W의 낮은 전력으로 5초간 산소 플라즈마 처리를 시행하는 것이 최적 조건이 었으며 슈퍼커패시터의 에너지 밀도가 약 8% 증가하였다.

Energy storage systems should address issues such as power fluctuations and rapid charge-discharge; to meet this requirement, CoFe2O4 (CFO) spinel nanoparticles with a suitable electrical conductivity and various redox states are synthesized and used as electrode materials for supercapacitors. In particular, CFO electrodes combined with carbon nanofibers (CNFs) can provide long-term cycling stability by fabricating binder-free three-dimensional electrodes. In this study, CFO-decorated CNFs are prepared by electrospinning and a low-cost hydrothermal method. The effects of heat treatment, such as the activation of CNFs (ACNFs) and calcination of CFO-decorated CNFs (C-CFO/ACNFs), are investigated. The C-CFO/ACNF electrode exhibits a high specific capacitance of 142.9 F/g at a scan rate of 5 mV/s and superior rate capability of 77.6% capacitance retention at a high scan rate of 500 mV/s. This electrode also achieves the lowest charge transfer resistance of 0.0063 Ω and excellent cycling stability (93.5% retention after 5,000 cycles) because of the improved ion conductivity by pathway formation and structural stability. The results of our work are expected to open a new route for manufacturing hybrid capacitor electrodes containing the C-CFO/ACNF electrode that can be easily prepared with a low-cost and simple process with enhanced electrochemical performance.

Hierarchically porous carbon materials with high nitrogen functionalities are extensively studied as highperformance supercapacitor electrode materials. In this study, nitrogen-doped porous carbon textile (N-PCT) with hierarchical pore structures is prepared as an electrode material for supercapacitors from a waste cotton T-shirt (WCT). Porous carbon textile (PCT) is first prepared from WCT by two-step heat treatment of stabilization and carbonization. The PCT is then nitrogendoped with urea at various concentrations. The obtained N-PCT is found to have multi-modal pore structures with a high specific surface area of 1,299 m2 g−1 and large total pore volume of 1.01 cm3 g−1. The N-PCT-based electrode shows excellent electrochemical performance in a 3-electrode system, such as a specific capacitance of 235 F g−1 at 1 A g−1, excellent cycling stability of 100 % at 5 A g−1 after 1,000 cycles, and a power density of 2,500 W kg−1 at an energy density of 3.593 Wh kg−1. Thus, the prepared N-PCT can be used as an electrode material for supercapacitors.

Porous carbons have been widely used as electrode material for supercapacitors. However, commercial porous carbons, such as activated carbons, have low electrochemical performance. Nitrogen-doping is one of the most promising strategies to improve electrochemical performance of porous carbons. In this study, nitrogen self-doped porous carbon (NPC) is prepared from melamine foam by carbonization to improve the supercapacitive performance. The prepared NPC is characterized in terms of the chemical structures and elements, morphology, pore structures, and electrochemical performance. The results of the N2 physisorption measurement, X-ray diffraction, and Raman analyses reveal that the prepared NPC has bimodal pore structures and pseudo-graphite structures with nitrogen functionality. The NPC-based electrode exhibits a gravimetric capacitance of 153 F g−1 at 1 A g−1, a rate capability of 73.2 % at 10 A g−1, and an outstanding cycling ability of 97.85% after 10,000 cycles at 10 A g−1. Thus, the NPC prepared in this study can be applied as electrode material for high-performance supercapacitors.

Electronic textiles promise to provide an intelligent platform to enlarge the scope of wearable electronic applications. Therefore, the combination of flexible energy storage devies into wearable systems is a key for operating these electronic textiles during bending, knotting, and rolling. Nonetheless, the application of fibrous supercapacitors consisting of a gel-electrolyte and carbon fiber electrode is still obstructed by low capacitance, low rate-performance, and poor cycling stability owing to the inefficient interface between the gel-electrolyte and electrode. Here, a fibrous supercapacitor is obtained using an optimized gelelectrolyte that improves the ionic diffusion capability. The optimized fibrous supercapacitor shows a superior electrochemical performance, including high specific capacitance of 41 mF cm−2 at current density of 2.0 μA cm−2, high-rate performance with 17 mF cm−2 at a current density of 15.0 μA cm−2, and outstanding cycling stability (88% after 3,000 cycles at a current density of 200.0 μA cm−2). The excellent energy storage performance is mainly attributed to the optimzied interface between the gelelectrolyte and electrode material, leading to an improved ionic diffusion capability.

본 연구에서는 다공성 활성탄소와 금속유기골격체 복합재료 기반의 전극 재료와 “이온젤” 이라고 불리는 고분자 고체 전해질을 이용하여 슈퍼커패시터를 제작 하였으며, 금속유기골격체의 함량에 따른 전기화학적 거동을 관찰하여 보았다. 슈퍼커패시터의 전기화학적 특성은 순환전압전류법(CV), 전기화학적 임피던스 분광법(EIS) 및 전정류 충·방전법(GCD)으로 분석하였으며, 그 결과로, 다공성 활성탄소 대비 금속유기골격체를 0.5 wt% 첨가 하였을 때 가장 높은 전기용량값을 확인 할 수 있었으며, 0.5 wt% 이상의 금속유기골격체의 함유량은 전기화학적 특성 감소에 영향을 주는 것으로 사료되며, 이러한 결과를 바탕으로 제조된 다공성 활성탄소/금속유기골격체 복합재료 기반의 슈퍼커패시터는 다양한 분야에 활용이 가능 할 것으로 판단된다.

Zinc-ion hybrid supercapacitors (ZICs) have recently been spotlighted as energy storage devices due to their high energy and high power densities. However, despite these merits, ZICs face many challenges related to their cathode materials, activated carbon (AC). AC as a cathode material has restrictive electrical conductivity, which leads to low capacity and lifetime at high current densities. To overcome this demerit, a novel boron (B) doped AC is suggested herein with improved electrical conductivity thanks to B-doping effect. Especially, in order to optimize B-doped AC, amounts of precursors are regulated. The optimized B-doped AC electrode shows a good charge-transfer process and superior electrochemical performance, including high specific capacity of 157.4 mAh g−1 at current density of 0.5 A g−1, high-rate performance with 66.6 mAh g−1 at a current density of 10 A g−1, and remarkable, ultrafast cycling stability (90.7 % after 10,000 cycles at a current density of 5 A g−1). The superior energy storage performance is attributed to the B-doping effect, which leads to an excellent charge-transfer process of the AC cathode. Thus, our strategy can provide a rational design for ultrafast cycling stability of next-generation supercapacitors in the near future.

The performance of Li-ion hybrid supercapacitors (asymmetric-type) depends on many factors such as the capacity ratio, material properties, cell designs and operating conditions. Among these, in consideration of balanced electrochemical reactions, the capacity ratio of the negative (anode) to positive (cathode) electrode is one of the most important factors to design the Li-ion hybrid supercapacitors for high energy storing performance. We assemble Li-ion hybrid supercapacitors using activated carbon (AC) as anode material, lithium manganese oxide as cathode material, and organic electrolyte (1 mol L−1 LiPF6 in acetonitrile). At this point, the thickness of the anode electrode is controlled at 160, 200, and 240 μm. Also, thickness of cathode electrode is fixed at 60 μm. Then, the effect of negative and positive electrode ratio on the electrochemical performance of AC/LiMn2O4 Li-ion hybrid supercapacitors is investigated, especially in the terms of capacity and cyclability at high current density. In this study, we demonstrate the relationship of capacity ratio between anode and cathode electrode, and the excellent electrochemical performance of AC/LiMn2O4 Li-ion hybrid supercapacitors. The remarkable capability of these materials proves that manipulation of the capacity ratio is a promising technology for high-performance Li-ion hybrid supercapacitors.

인류의 에너지 수급은 항상 인간의 삶에 중요한 문제이며, 최근에는 전기 생산 및 공급 문제로 이어지고 있다. 이에 관련하여 본 연구에서는 에너지 저장장치의 일환으로 슈퍼커패시터 용도의 고체 전해질막을 제조하였다. 제조한 전해질막 은 poly(vinyl alcohol) (PVA) 주사슬에 poly(oxyethylene methacrylate) (POEM) 곁사슬을 그래프팅하여 사용하였으며, 그래프팅은 자유 라디칼 중합법을 통해 합성하였다. 본 연구에서 사용한 PVA-g-POEM 가지형 공중합체를 슈퍼커패시터 전해질에 적용한 사례는 처음이다. POEM 그래프팅을 통해 PVA가 고유하게 가지고 있던 구조가 변화하였으며, 이를 FT-IR을 통해 분석하였다. 또한, 합성한 공중합체를 이용한 슈퍼커패시터 성능은 cyclic voltammetry (CV), galvanostatic charge/discharge (GCD), ragone plot 등을 통해 분석하였다. 이를 통해 기존에 수계 전해질로 PVA 단일 고분자만 사용하던 분야에 그래프팅 방법이라는 새로운 접근법을 제시하였다.

본 연구에서는 “이온젤” 이라고 불리는 고분자 기반의 PVA(polyvinyl alcohol)-H₃PO₄의 고체 전해질에 이온성 액체 BMIMBF4 (1-buthyl-3-methylimidazolium tetrafluoroborate)를 첨가하여 제조한 전고체 전해질과 환원된 그래핀 옥사이드/전도성 고분자 복합재료 기반의 전극 재료를 이용하여 유연성을 갖는 슈퍼커패시터를 제작 하였으며, 유연성에 따른 전기화학적 특성을 분석하여 보았다. 환원된 그래 핀 옥사이드/전도성 고분자 복합재료와 전고체 전해질 기반의 유연성 슈퍼커패시터의 전기화학적 특성을 유연성에 따라서 측정하기 위해서 프레스로 0.01 kg/cm²의 일정한 압력으로 최대 100회 까지 굽힘 시험 (bending test)을 진행 하였으며, 0~100 회의 굽힘 시험 이후에 순환 전압전류법(CV), 전기화학적 임피던스 분광법(EIS) 및 전정류 충·방전법(GCD)을 통하여 비교 및 분석하여 보았다. 그 결과로, 유연성 슈퍼커 패시터의 초기 전기용량은 43.9 F/g으로 확인 할 수 있었고, 이 값은 50회, 100회의 굽힘 시험 후에 각각 42.0F/g, 40.1F/g로 감소하는 현상을 확인할 수 있었다. 이러한 결과로 미루어 보아 물리적인 응력이 슈퍼 커패시터의 전기화학적 특성 감소에 영향을 주는 것으로 사료되며 또한, 굽힘 횟수에 따른 슈퍼커패시터의 전기화학적 특성 감소 원인을 확인하기 위해서 굽힘 시험 전과 후의 전극표면을 전자주사 현미경으로 관찰 하여 보았다.

본 연구에서는 탄소 나노재료 중 환원된 그래핀 옥사이드와 전도성 고분자중 폴리아닐린을 복합화 하여 슈퍼커패시터용 전극을 제조하였으며, 각각의 전극 재료가 가지는 단점을 서로 보완하고 장점을 극대화시킴으로써 전극의 전기화학적 특성을 크게 향상 시킬 수 있었다. 전극 물질에 사용된 폴리아닐린은 아닐린 단량체를 화학 중합법으로 제조하였고, 환원된 그래핀 옥사이드는 별도의 전 처리 과정 없이 사용 하였으며, DMF(N,N-dimethyl formamide)를 용매로 도입하여 분산용액을 제조하였다. 분산용액은 금이 코팅된PET(Polyethylene terephthalate) 기판위에 산업적 스케일로 적용이 가능한 스프레이 코팅 방법을 이용하여 전극으로 제조하였다. 환원된 그래핀 옥사이드/폴리아닐린 복합재료를 기반으로 제조된 전극의 전기화학적 특성을 비교하기 위하여 환원된 그래핀 옥사이드와 폴리아닐린 단일 전극을 제조하였으며, 동일 한 조건하에서 순환전압전류법, 임피던스 분광법, 정전류 충·방전법을 통하여 각각의 전극이 나타내는 전기 화학적 특성을 비교·분석 하였다. 그 결과로, 환원된 그래핀 옥사이드/폴리아닐린 복합재료를 기반으로 제조된 전극은 폴리아닐린, 환원된 그래핀 옥사 단일 전극에 비하여 전기 용량 값이 높게 나타났으며, 전해질 계면과의 내부 저항은 폴리아닐린, 환원된 그래핀 옥사이드 단일 전극에 비하여 각각 24 %, 58 % 감소하는 결과를 나타내었다. 이러한 결과로 미루어보아 본 연구를 통하여 제조된 환원된 그래핀 옥사이드/폴리 아닐린 복합재료 기반의 전극은 유연성 에너지 저장 매체나 웨어러블 전자기기에 적용이 가능할 것으로 판단된다.

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.