Improving the electrochemical performances of active carbon-based supercapacitors through the combination of introducing functional groups and using redox additive electrolyte

High-performance and low-cost electrochemical capacitors (ECs) are essential for large-scale applications in energy storage. In this work, the specific capacitance of active carbon (AC) electrode was significantly improved through the combination of introducing functional groups on the surface of AC and adding redox-active molecules (K₃Fe(CN)₆) into 2?M KOH aqueous electrolytes. The surface-oxygen functionalized AC (FAC) was synthesized using HNO₃ echoed as the electrode and 2?M KOH with 0.1?M K₃Fe(CN)₆ as the electrolyte. The surface functional groups of the AC not only contribute to the pseudocapacitance but also increase the active sites of the electrode/electrolyte interface, which enhances the electrochemical activity of the Fe(CN)₆^3?/Fe(CN)₆^4? redox pair, thus leading to high capacitance. In the redox electrolyte, the specific capacitance was much higher in 229.17?F?g^?1 (1?A?g^?1) achieved for those FAC than in raw AC (only 147.06?F?g^?1). Similarly, the FAC electrode suggested high energy density and extended cycling stability in the KOH?+?K₃Fe(CN)₆ electrolyte.     

Electrochemical performance of metal-organic framework synthesized by a solvothermal method for supercapacitors

A series of metal-organic frameworks (MOFs) based on isonicotinic acid and nickel nitrate were successfully synthesized by a solvothermal method as electrode materials for supercapacitor. The MOF were examined by X-ray diffraction (XRD) patterns and N₂ adsorption/desorption isotherms. Electrochemical properties of the materials were characterized by cyclic voltammetry (CV) in 6 M KOH aqueous solutions. The effect of solvothermal time, temperature and the mol ratio of isonicotinic acid and nickel nitrate on the electrochemical performance were also studied. The maximum specific capacitance is found to be 634 F g^?1 at 5 mV s^?1 and the stable cycling properties measurement showed the sample kept 84% after 2000 cycles at a 50 mV s^?1 scan rate.     

Supercapacitive behaviors of the nitrogen-enriched activated mesocarbon microbead in aqueous electrolytes

The activated nitrogen-enriched novel carbons (a-NENCs) have been prepared by direct carbonization of polyaniline/activated mesocarbon microbead composites and further activated by 16 M?HNO₃. The electrochemical performances and supercapacitive behaviors of the a-NENCs in 6 M KOH, 1 M?H₂SO₄, and 0.5 M?K₂SO₄ solutions are evaluated by cyclic voltammetry, galvanostatic charge/discharge, electrochemical impedance spectroscopy, cyclic life, leakage current, and self-discharge measurements. The results demonstrate that the supercapacitors perform definitely supercapacitive behaviors; especially in 6 M KOH electrolyte, the supercapacitor represents much better electrochemical performance with more excellent reversibility, shorter relaxation time of 1.11 s, and nearly ideal polarizability. The maximum specific capacitance of the supercapacitors using a-NENCs as active electrode material is 85.1 F?g^?1 at a rate of 500 mA?g^?1 in 6 M?KOH. These outcomes indicate that the 6 M?KOH aqueous solution is a promising electrolyte for the supercapacitor with a-NENCs as electrode material.     

Nitrogen‐Doped Porous Graphitic Carbon as an Excellent Electrode Material for Advanced Supercapacitors

An advanced supercapacitor material based on nitrogen‐doped porous graphitic carbon (NPGC) with high a surface area was synthesized by means of a simple coordination–pyrolysis combination process, in which tetraethyl orthosilicate (TEOS), nickel nitrate, and glucose were adopted as porogent, graphitic catalyst precursor, and carbon source, respectively. In addition, melamine was selected as a nitrogen source owing to its nitrogen‐enriched structure and the strong interaction between the amine groups and the glucose unit. A low‐temperature treatment resulted in the formation of a NPGC precursor by combination of the catalytic precursor, hydrolyzed TEOS, and the melamine–glucose unit. Following pyrolysis and removal of the catalyst and porogent, the NPGC material showed excellent electrical conductivity owing to its high crystallinity, a large Brunauer–Emmett–Teller surface area (S_BET=1027 m² g^?1), and a high nitrogen level (7.72 wt %). The unusual microstructure of NPGC materials could provide electrochemical energy storage. The NPGC material, without the need for any conductive additives, showed excellent capacitive behavior (293 F g^?1 at 1 A g^?1), long‐term cycling stability, and high coulombic efficiency (>99.9 % over 5000 cycles) in KOH when used as an electrode. Notably, in a two‐electrode symmetric supercapacitor, NPGC energy densities as high as 8.1 and 47.5 Wh kg^?1, at a high power density (10.5 kW kg^?1), were achieved in 6 M KOH and 1 M Et₄NBF₄‐PC electrolytes, respectively. Thus, the synthesized NPGC material could be a highly promising electrode material for advanced supercapacitors and other conversion devices.     

Core–Shell Carbon‐Coated CuO Nanocomposites: A Highly Stable Electrode Material for Supercapacitors and Lithium‐Ion Batteries

Herein we present a simple method for fabricating core–shell mesostructured CuO@C nanocomposites by utilizing humic acid (HA) as a biomass carbon source. The electrochemical performances of CuO@C nanocomposites were evaluated as an electrode material for supercapacitors and lithium‐ion batteries. CuO@C exhibits an excellent capacitance of 207.2 F g^?1 at a current density of 1 A g^?1 within a potential window of 0–0.46 V in 6 M KOH solution. Significantly, CuO electrode materials achieve remarkable capacitance retentions of approximately 205.8 F g^?1 after 1000 cycles of charge/discharge testing. The CuO@C was further applied as an anode material for lithium‐ion batteries, and a high initial capacity of 1143.7 mA h g^?1 was achieved at a current density of 0.1 C. This work provides a facile and general approach to synthesize carbon‐based materials for application in large‐scale energy‐storage systems.     

A hexaazatriphenylene-based porous organic polymer for high performance supercapacitor

Porous organic polymers (POPs) with high physiochemical stability and pseudocapacitive activity are crucial for supercapacitors with high specific capacitance and long cycle life. We report herein a hexaazatrinaphthylene-based POP (HPOP-1) for high-performance supercapacitor by introducing redox-active hexaazatrinaphthylene (HATN) moiety through Sonogashira–Hagihara coupling reaction. HATN moiety can undergo a proton-induced electron transfer redox reaction, which endows HPOP-1 with high pseudocapacitive activity. As electrode materials for supercapacitor application, HPOP-1 exhibits high specific capacitance (667 F g⁻¹ at 0.5 A g⁻¹) and long-term cyclic stability (90% capacitance retention after 10,000 cycles at 5 A g⁻¹) in a three-electrode system with 1 M H₂SO₄ as the electrolyte. In addition, HPOP-1 also exhibits a specific capacitance of 376 F g⁻¹ at 0.5 A g⁻¹ in 1 M KOH electrolyte. An asymmetric supercapacitor was further fabricated with HPOP-1 as negative electrode and rGO as positive electrode, respectively. The device delivers a specific capacitance of 63 F g⁻¹ at 0.5 A g⁻¹ and a rate performance of 37 F g⁻¹ at 5 A g⁻¹. Our work provides a facile approach for the design and preparation of pseudocapacitive POPs with high specific capacitance and long cycle life.     

Ultrahigh Energy Density Realized by a Single‐Layer β‐Co(OH)2 All‐Solid‐State Asymmetric Supercapacitor

A conceptually new all‐solid‐state asymmetric supercapacitor based on atomically thin sheets is presented which offers the opportunity to optimize supercapacitor properties on an atomic level. As a prototype, β‐Co(OH)₂ single layers with five‐atoms layer thickness were synthesized through an oriented‐attachment strategy. The increased density‐of‐states and 100 % exposed hydrogen atoms endow the β‐Co(OH)₂ single‐layers‐based electrode with a large capacitance of 2028 F g^?1. The corresponding all‐solid‐state asymmetric supercapacitor achieves a high cell voltage of 1.8 V and an exceptional energy density of 98.9 Wh kg^?1 at an ultrahigh power density of 17 981 W kg^?1. Also, this integrated nanodevice exhibits excellent cyclability with 93.2 % capacitance retention after 10 000 cycles, holding great promise for constructing high‐energy storage nanodevices.     

Hierarchical Activated Mesoporous Phenolic‐Resin‐Based Carbons for Supercapacitors

A series of hierarchical activated mesoporous carbons (AMCs) were prepared by the activation of highly ordered, body‐centered cubic mesoporous phenolic‐resin‐based carbon with KOH. The effect of the KOH/carbon‐weight ratio on the textural properties and capacitive performance of the AMCs was investigated in detail. An AMC prepared with a KOH/carbon‐weight ratio of 6:1 possessed the largest specific surface area (1118 m² g^?1), with retention of the ordered mesoporous structure, and exhibited the highest specific capacitance of 260 F g^?1 at a current density of 0.1 A g^?1 in 1 M H₂SO₄ aqueous electrolyte. This material also showed excellent rate capability (163 F g^?1 retained at 20 A g^?1) and good long‐term electrochemical stability. This superior capacitive performance could be attributed to a large specific surface area and an optimized micro‐mesopore structure, which not only increased the effective specific surface area for charge storage but also provided a favorable pathway for efficient ion transport.     

Hierarchically Porous Nickel Oxide Nanosheets Grown on Nickel Foam Prepared by One‐Step In Situ Anodization for High‐Performance Supercapacitors

Porous NiO nanosheets are successfully grown on nickel foam substrate through an in situ anodization by using molten KOH as the electrolyte. High‐purity NiO is directly obtained by this one‐step method without any subsequent treatment. The obtained NiO supported on nickel foam is used as a binder‐free electrode for a supercapacitor and its pseudocapacitive behavior has been investigated by cyclic voltammetry and galvanostatic charge–discharge tests in a 6 M aqueous solution of KOH. Electrochemical data demonstrates that this binder‐free electrode possesses ultrahigh capacitance (4.74 F cm^?2 at 4 mA cm^?2), excellent rate capability, and cycling stability. After 1000 cycles, the areal capacitance value is 9.4 % lower than the initial value and maintains 85.4 % of the maximum capacitance value.     

A Reversible Redox Strategy for SWCNT‐Based Supercapacitors Using a High‐Performance Electrolyte

In order to achieve pesudocapacitive performance of single‐wall carbon nanotube (SWCNT) electrodes, a high‐efficient and reversible redox strategy utilizing a redox‐mediated electrolyte for SWCNT‐based supercapacitors is reported. In this novel redox‐mediated electrolyte, the single‐electrode specific capacitance of the supercapacitor is heightened four times, reaching C=162.66 F g^?1 at 1 A g^?1. The quick charge‐discharge ability of the supercapacitor is also enhanced, and the relaxation time is as low as 0.58 s. Furthermore, the supercapacitor shows an excellent cycling performance of 96.51 % retention after 4000 cycles. The remarkable results presented here illustrate that the redox strategy is a facile and straightforward approach to improve the performances of SWCNT electrodes.     

Constant current anodic stripping chronopotentiometric determination of uranium in uranium mineral ores via accumulation of K<Subscript>2</Subscript>UO<Subscript>2</Subscript>[Fe(CN)<Subscript>6</Subscript>] on the palladium plated aluminum electrode

In the present work the uranyl hexacyanoferrate (K₂UO₂[Fe(CN)₆]) is deposited on the palladized aluminum (Pd-Al) electrode from a \textUO₂^{2 +} + \textFe( \textCN )₆ ^{- 3} {\text{UO}}_{2}^{2 + } + {\text{Fe}}\left( {\text{CN}} \right)_{6}^{ - 3} solution. Then the anodic stripping chronopotentiometry (ASCP) was used to strip the K₂UO₂[Fe(CN)₆] from the Pd-Al surface. The operational conditions including: pH, K₃Fe(CN)₆ concentration, deposition potential, deposition time and stripping current were optimized. The ASCP calibration graph was linear in concentration range 10–460 μM. of \textUO₂^{2 +} {\text{UO}}_{2}^{2 + } and the detection limit was 8.5 μM. The interference of some concomitant ions during the deposition process of K₂UO₂[Fe(CN)₆] was studied. The proposed method was successfully applied for analysis of some uranium mineral ores.     

Electrodeposited PbO2 thin film on Ti electrode for application in hybrid supercapacitor

PbO₂ thin films were prepared by pulse current technique on Ti substrate from Pb(NO₃)₂ plating solution. The hybrid supercapacitor was designed with PbO₂ thin film as positive electrode and activated carbon (AC) as negative electrode in the 5.3 M H₂SO₄ solution. Its electrochemical properties were determined by cyclic voltammetry (CV), charge–discharge test and electrochemical impedance spectroscopy (EIS). The results revealed that the PbO₂/AC hybrid supercapacitor exhibited large specific capacitance, high-power and stable cycle performance. In the potential range of 0.8–1.8 V, the hybrid supercapacitor can deliver a specific capacitance of 71.5 F g^?1 at a discharge current density of 200 mA g^?1(4 mA cm^?2) when the mass ratio of AC to PbO₂ was three, and after 4500 deep cycles, the specific capacitance remains at 64.4 F g^?1, or 32.2 Wh Kg^?1 in specific energy, and the capacity only fades 10% from its initial value.     

Perovskite SrCo0.9Nb0.1O3−δ as an Anion‐Intercalated Electrode Material for Supercapacitors with Ultrahigh Volumetric Energy Density

We have synthesized and characterized perovskite‐type SrCo_0.9Nb_0.1O_3−δ (SCN) as a novel anion‐intercalated electrode material for supercapacitors in an aqueous KOH electrolyte, demonstrating a very high volumetric capacitance of about 2034.6 F cm⁻³ (and gravimetric capacitance of ca. 773.6 F g⁻¹) at a current density of 0.5 A g⁻¹ while maintaining excellent cycling stability with a capacity retention of 95.7 % after 3000 cycles. When coupled with an activated carbon (AC) electrode, the SCN/AC asymmetric supercapacitor delivered a specific energy density as high as 37.6 Wh kg⁻¹ with robust long‐term stability.     

Preparation and performance of polyvinyl alcohol-based activated carbon as electrode material in both aqueous and organic electrolytes

Porous carbon materials with high surface area and different pore structure have been successfully prepared by phenolic resin combined with polyvinyl alcohol (PVA) and KOH as activation agents. The surface morphology, structure, and specific surface area of the carbon materials were studied by scanning electron microscopy, X-ray diffraction, and nitrogen sorption measurement, respectively. Furthermore, the effects of specific surface area, pore structure, and electrolyte on electrochemical properties were investigated by galvanostatic charge–discharge measurement. The results show that KOH–PVA-activated carbon materials display specific capacitance as high as 218 F?g^?1 in 30 wt.% KOH aqueous electrolyte, 147 F?g^?1 in 1 M LiPF₆/(ethylene carbonate (EC) + dimethyl carbonate) (1:1?v/v), and 115 F?g^?1 in 1 M Et₃MeNBF₄/propylene carbonate organic electrolyte, respectively. In addition, the carbon materials demonstrate long-term cycle stability, especially the AK3P-0.30 in aqueous electrolyte and the AK2P-0.30 with excellent rate capability in organic electrolyte. These reveal that the existence of a micro-mesoporous structure of activated carbon is beneficial to store energy in an aqueous supercapacitor and broad pore size distribution of activated carbon is favorable to energy storage in an organic supercapacitor. The carbon materials with pore size distribution in different ranges improve the electrochemical performance of supercapacitor in different electrolytes. A new pore-expand agent (PVA combining with KOH) was used to obtain porous carbons with enhanced properties for supercapacitor.     

KOH‐Activated Porous Carbons Derived from Chestnut Shell with Superior Capacitive Performance

Porous carbons (PC) were prepared from a waste biomass named chestnut shell via a two‐step method involving carbonization and KOH activation. The morphology, pore structure and surface chemical properties were investigated by scanning electron microscopy (SEM), N₂ sorption, Raman spectroscopy, X‐ray diffraction (XRD) and X‐ray photoelectron spectroscopy (XPS). The carbons have been evaluated as the electrode materials for supercapacitors by a two‐electrode system in 6 mol/L KOH electrolyte. Benefiting from the porous texture, high surface area and high oxygen content, the PCs derived from chestnut shell have exhibited high specific capacitance of 198.2 (PC‐1), 217.2 (PC‐2) and 238.2 F·g^?1 (PC‐3) at a current density of 0.1 A·g^?1, good rate capability of 55.7%, 56.6% and 54.9% in a range of 0.1–20 A·g^?1 and high energy density of 5.6, 6.1 and 6.7 Wh·kg^?1, respectively. This is believed to be due to electric double layer capacitance induced by the abundant micropores and extra pseudo‐capacitance generated by oxygen‐containing groups. At a power density of 9000 Wh·kg^?1, the energy density is 3.1, 3.5 and 3.7 Wh·kg^?1 for PC‐1, PC‐2 and PC‐3, respectively, demonstrating the potential of the carbons derived from chestnut shells in energy storage devices.     

Controlling the BET Surface Area of Porous Carbon by Using the Cd/C Ratio of a Cd–MOF Precursor and Enhancing the Capacitance by Activation with KOH

Herein, four new cadmium metal–organic frameworks (Cd–MOFs), [Cd(bib)(bdc)]_∞ ( 1 ), [Cd(bbib)(bdc)(H₂O)]_∞ ( 2 ), [Cd(bibp)(bdc)]_∞ ( 3 ), and [Cd₂(bbibp)₂(bdc)₂(H₂O)]_∞ ( 4 ), have been constructed from the reaction of Cd(NO₃)₂ ? 4 H₂O with 1,4‐benzenedicarboxylate (H₂bdc) and structure‐related bis(imidazole) ligands (1,4‐bis(imidazol‐1‐yl)benzene (bib), 1,4‐bis(benzoimidazol‐1‐yl)benzene (bbib), 4,4′‐bis(imidazol‐1‐yl)biphenyl (bibp), and 4,4′‐bis(benzoimidazol‐1‐yl)biphenyl (bbibp)) under solvothermal conditions. Cd–MOF 1 shows a 2D (4,4) lattice with parallel interpenetration, whereas 2 displays an interesting 3D interpenetrating dia network, 3 exhibits an unusual 3D interpenetrating dmp network, and 4 presents a 3D self‐catenated pillar‐layered framework with a Schäfli symbol of [4³ ? 6³]₂ ? [4⁶ ? 6¹⁶ ? 8⁶]. The structural diversity indicates that the backbone of the bis(imidazole) ligand (including the terminal group and spacer) plays a crucial role in the assembly of mixed‐ligand frameworks. By using the pore‐forming effect of cadmium vapor, for the first time we have utilized these Cd–MOFs as precursors to further prepare porous carbon materials (PCs) in a calcination–thermolysis procedure. These PCs show different porous features that correspond to the topological structures of Cd–MOFs. Significantly, it was found that the specific surface area and capacitance of PCs are tuned by the Cd/C ratio of the MOF. Furthermore, the as‐synthesized PCs were processed with KOH to obtain activated porous carbon materials (APCs) with higher specific surface area and porosity, which greatly promoted the energy‐storage capacity. After full characterization, we found that APC‐bib displays the largest specific surface area (1290 m² g^?1) and total pore volume (1.37 cm³ g^?1) of this series of carbon materials. Consequently, APC‐bib demonstrates the highest specific capacitance of 164 F g^?1 at a current density of 0.5 A g^?1, and also excellent retention of capacitance (≈89.4 % after 5000 cycles at 1 A g^?1). Therefore, APC‐bib has great potential as the electrode material in a supercapacitor.     

Synthesis of Hierarchically Porous Sandwich‐Like Carbon Materials for High‐Performance Supercapacitors

For the first time, hierarchically porous carbon materials with a sandwich‐like structure are synthesized through a facile and efficient tri‐template approach. The hierarchically porous microstructures consist of abundant macropores and numerous micropores embedded into the crosslinked mesoporous walls. As a result, the obtained carbon material with a unique sandwich‐like structure has a relatively high specific surface (1235 m² g^?1), large pore volume (1.30 cm³ g^?1), and appropriate pore size distribution. These merits lead to a comparably high specific capacitance of 274.8 F g^?1 at 0.2 A g^?1 and satisfying rate performance (87.7 % retention from 1 to 20 A g^?1). More importantly, the symmetric supercapacitor with two identical as‐prepared carbon samples shows a superior energy density of 18.47 Wh kg^?1 at a power density of 179.9 W kg^?1. The asymmetric supercapacitor based on as‐obtained carbon sample and its composite with manganese dioxide (MnO₂) can reach up to an energy density of 25.93 Wh kg^?1 at a power density of 199.9 W kg^?1. Therefore, these unique carbon material open a promising prospect for future development and utilization in the field of energy storage.     

Three‐Dimensional Nitrogen‐Doped Hierarchical Porous Carbon as an Electrode for High‐Performance Supercapacitors

A facile and sustainable procedure for the synthesis of nitrogen‐doped hierarchical porous carbons with a three‐dimensional interconnected framework (NHPC‐3D) was developed. The strategy, based on a colloidal crystal‐templating method, utilizes nitrogenous dopamine as the precursor due to its unique properties, including self‐polymerization under mild alkaline conditions, coating onto various surfaces, a high carbonization yield, and well‐preserved nitrogen doping after heat treatment. The obtained NHPC‐3D possesses a high surface area of 1056 m² g^?1, a large pore volume of 2.56 cm³ g^?1, and a high nitrogen content of 8.2 wt %. The NHPC‐3D is implemented as the electrode material of a supercapacitor and exhibits a specific capacitance as high as 252 F g^?1 at a current density of 2 A g^?1. The device also shows a high capacitance retention of 75.7 % at a higher current density of 20 A g^?1 in aqueous electrolyte due to a sufficient surface area for charge accommodation, reversible pseudocapacitance, and minimized ion‐transport resistance, as a result of the advantageous interconnected hierarchical porous texture. These results showcase NHPC‐3D as a promising candidate for electrode materials in supercapacitors.     

Preparation of a NiAl‐Oxide@Polypyrrole Composite for High‐Performance Supercapacitors

A core‐shell NiAlO@polypyrrole composite (NiAlO@PPy) with a 3D “sand rose”‐like morphology was prepared via a facile in situ oxidative polymerization of pyrrole monomer, where the role of PPy coating thickness was investigated for high‐performance supercapacitors. Microstructure analyses indicated that the PPy was successfully coated onto the NiAlO surface to form a core‐shell structure. The NiAlO@PPy exhibited a better electrochemical performance than pure NiAlO, and the moderate thickness of the PPy shell layer was beneficial for expediting the electron transfer in the redox reaction. It was found that the NiAlO@PPy₅ prepared at 5.0 mL L^?1 addition amount of pyrrole monomer demonstrated the best electrochemical performance with a high specific capacitance of 883.2 F g^?1 at a current density of 1 A g^?1 and excellent capacitance retention of 91.82 % of its initial capacitance after 1000 cycles at 3 A g^?1. The outstanding electrochemical performance of NiAlO@PPy₅ were due to the synergistic effect of NiAlO and PPy, where the uniform network‐like PPy shell with the optimal thickness made electrolyte ions more easily accessible for faradic reactions. This work provided a simple approach for designing organic–inorganic core‐shell materials as high‐performance electrode materials for electrochemical supercapacitors.     

Synthesis of micro- and mesoporous carbon spheres for supercapacitor electrode

Micro- and mesoporous carbon spheres (MMCSs) are synthesized by the polymerization of colloidal silica-entrapped resorcinol/formaldehyde in the presence of ammonia as catalyst, followed by carbonization, sodium hydroxide (NaOH) etching to remove silica template, and potassium hydroxide (KOH) activation. The morphology and microstructure are characterized by scanning electron microscopy, transmission electron microscopy, and nitrogen adsorption–desorption. The results show that a typical sample (denoted as MMCS-3) unites the characteristics of regular spherical shape (uniform diameters of 500 nm), high specific surface area (1,620 m² g^?1), large pore volume (1.037 cm³ g^?1), and combined micropores and mesopores (11.0 nm), which endows MMCS-3 good electrochemical performance. MMCS-3 as supercapacitor electrode shows a specific capacitance of 314 F g^?1 under a current density of 0.5 A g^?1 and low internal resistance of 0.2 Ω in 6 M KOH aqueous solution. The electrochemical capacitance still retains 198 F g^?1 at a high current density of 10 A g^?1. After 500 cycle numbers of galvanostatic charge/discharge at 0.5 A g^?1, MMCS-3 electrode still remains the specific capacitance of 301 F g^?1 with the retention of 96 %. This study highlights the potential of well-designed MMCSs as electrodes for widespread supercapacitor applications.