Carbon Nanotube@N‐Doped Mesoporous Carbon Composite Material for Supercapacitor Electrodes

Here, carbon nanotube@N‐doped mesoporous carbon (CNT@N‐PC) composites were synthesized by using resorcinol‐formaldehyde resin as carbon source, ionic liquids (ILs) as template, and nitrogen sources and tetraethyl orthosilicate (TEOS) as assistant agent. The use of ILs‐modified CNT with nitrogen and TEOS facilitated the generation of a richer mesoporous structure. The obtained CNT@N‐PC was composed of a CNT core and mesoporous carbon particles around it. CNT@N‐PC showed a 3D network structure like “dewy cobwebs” and had a high surface area of 857 m² g^?1, uniform pore size distribution (3.0 nm), and suitable N content (4.9 at.%). When used as supercapacitor electrode, the CNT@N‐PC exhibited a high specific capacitance (244 F g^?1 at 1 A g^?1), good rate capability and favorable capacitance retention (92.5 % capacitive retention after 5000 cycles), demonstrating the potential for application in high‐performance supercapacitors.     

Physical and electrochemical characterization of activated carbons with high mesoporous ratio for supercapacitors based on ionic liquid as the electrolyte

A series of activated carbons with high mesoporous ratio were prepared by KOH reactivation based on activated carbon as the precursor. As the KOH/AC mass ratio was increased to 4:1, the mesoporous ratio increases from 60% to 76%, and the average pore size from 2.23 to 3.14?nm. Moreover, the specific capacitance for the activated carbon in ionic liquid 1-ethyl-3-methylmidazolium tetrafluoroborate ([EMIm]BF₄) can reach the maximum value of 189?F?g^?1 (8.0???F?cm^?2). In addition, the decrease of specific capacitance for activated carbons by KOH reactivation with current density increase shows two regimes, suggesting that activated carbons with high mesoporous ratio are much fit for charge?Cdischarge at larger current density.     

Capacitive Properties of the Binder‐Free Electrode Prepared from Carbon Derived from Cotton and Reduced Graphene Oxide

The binder‐free composite films of reduced graphene oxide (rGO ) and activated carbon derived from cotton (aCFC ) have been fabricated and used as electrodes for electrochemical capacitors (ECs ) to avoid the decrease of capacitive performance in traditional process caused by the additional binder. The optimal aCFC is prepared at 850 °C when the mass ratio of carbon and potassium hydroxide is 1 to 4. The optimal composite film prepared from the mass ratio of aCFC /GO =2/1 exhibits porous structure, and has a specific surface area of 849.6 m²•g⁻¹ and a total pore volume of 0.61 mL •g⁻¹. Based on the two‐electrode system testing in 6.0 mol/L KOH electrolyte, the optimal composite has specific capacitance of about 202 F•g⁻¹, 374 mF •cm⁻² and 116 F•cm⁻³ in terms of mass, area and volume, and shows excellent rate capability and good cyclic stability (91.7% retention of the initial capacitance after 5000 cycles). Furthermore, the assembled solid‐state ECs by using KOH /polyvinyl alcohol as electrolyte show good mechanical stability and capacitive performances after repeated bending cycles. It is proved that this method is effective to fabricate binder‐free electrodes for ECs and will open up a novel route for the reuse of waste cotton.     

Synthesis of High‐Surface‐Area Nitrogen‐Doped Porous Carbon Microflowers and Their Efficient Carbon Dioxide Capture Performance

Sustainable carbon materials have received particular attention in CO₂ capture and storage owing to their abundant pore structures and controllable pore parameters. Here, we report high‐surface‐area hierarchically porous N‐doped carbon microflowers, which were assembled from porous nanosheets by a three‐step route: soft‐template‐assisted self‐assembly, thermal decomposition, and KOH activation. The hydrazine hydrate used in our experiment serves as not only a nitrogen source, but also a structure‐directing agent. The activation process was carried out under low (KOH/carbon=2), mild (KOH/carbon=4) and severe (KOH/carbon=6) activation conditions. The mild activated N‐doped carbon microflowers (A‐NCF‐4) have a hierarchically porous structure, high specific surface area (2309 m² g^?1), desirable micropore size below 1 nm, and importantly large micropore volume (0.95 cm³ g^?1). The remarkably high CO₂ adsorption capacities of 6.52 and 19.32 mmol g^?1 were achieved with this sample at 0 °C (273 K) and two pressures, 1 bar and 20 bar, respectively. Furthermore, this sample also exhibits excellent stability during cyclic operations and good separation selectivity for CO₂ over N₂.     

Heteroatom‐Doped Porous Carbon Nanosheets: General Preparation and Enhanced Capacitive Properties

High‐performance electrical double‐layer capacitors (EDLCs) require carbon electrode materials with high specific surface area, short ion‐diffusion pathways, and outstanding electrical conductivity. Herein, a general approach combing the molten‐salt method and chemical activation to prepare N‐doped carbon nanosheets with high surface area (654 m² g^?1) and adjustable porous structure is presented. Owing to their structural features, the N‐doped carbon nanosheets exhibited superior capacitive performance, demonstrated by a maximum capacitance of 243 F g^?1 (area‐normalized capacitance up to 37 μF cm^?2) at a current density of 0.5 A g^?1 in aqueous electrolyte, high rate capability (179 F g^?1 at 20 A g^?1), and excellent cycle stability. This method provides a new route to prepare porous and heteroatom‐doped carbon nanosheets for high‐performance EDLCs, which could also be extended to other polymer precursors and even waste biomass.     

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.     

Excellent Capacitive Performance of a Three‐Dimensional Hierarchical Porous Graphene/Carbon Composite with a Superhigh Surface Area

Three‐dimensional hierarchical porous graphene/carbon composite was successfully synthesized from a solution of graphene oxide and a phenolic resin by using a facile and efficient method. The morphology, structure, and surface property of the composite were investigated intensively by a variety of means such as scanning electron microscopy (SEM), transmission electron microscopy (TEM), N₂ adsorption, Raman spectroscopy, and Fourier transform infrared spectroscopy (FTIR). It is found that graphene serves as a scaffold to form a hierarchical pore texture in the composite, resulting in its superhigh surface area of 2034 m²g^?1, thin macropore wall, and high conductivity (152 S m^?1). As evidenced by electrochemical measurements in both EMImBF₄ ionic liquid and KOH electrolyte, the composite exhibits ideal capacitive behavior, high capacitance, and excellent rate performance due to its unique structure. In EMImBF₄, the composite has a high energy density of up to 50.1 Wh kg^?1 and also possesses quite stable cycling stability at 100 °C, suggesting its promising application in high‐temperature supercapacitors. In KOH electrolyte, the specific capacitance of this composite can reach up to an unprecedented value of 186.5 F g^?1, even at a very high current density of 50 A g^?1, suggesting its prosperous application in high‐power applications.     

Facile Synthesis of A 3D Flower‐Like Mesoporous Ni@C Composite Material for High‐Energy Aqueous Asymmetric Supercapacitors

A 3D flower‐like mesoporous Ni@C composite material has been synthesized by using a facile and economical one‐pot hydrothermal method. This unique 3D flower‐like Ni@C composite, which exhibited a high surface area (522.4 m² g^?1), consisted of highly dispersed Ni nanoparticles on mesoporous carbon flakes. The effect of calcination temperature on the electrochemical performance of the Ni@C composite was systematically investigated. The optimized material (Ni@C 700) displayed high specific capacity (1306 F g^?1 at 2 A g^?1) and excellent cycling performance (96.7 % retention after 5000 cycles). Furthermore, an asymmetric supercapacitor (ASC) that contained Ni@C 700 as cathode and mesoporous carbon (MC) as anode demonstrated high energy density (60.4 W h kg^?1 at a power density of 750 W kg^?1).     

Facile synthesis of biomass-derived hierarchical porous carbon microbeads for supercapacitors

Using the facile method of solvent evaporation, the leonardite fulvic acids (LFA)-based porous carbon microbeads (PCM) have been successfully prepared at ambient pressure, followed by carbonization and KOH activation (a low mass ratio alkali/LFA = 1.5) in an inert atmosphere. The effects of KOH treatment on pore structures and the formation mechanism of the PCM were discussed. The results showed that the sample exhibited remarkable improvement in textural properties. The activated carbon microbeads had high surface area (2269 m² g^?1), large pore volume (1.97 cm³ g^?1), and displayed excellent capacitive performances, compared with carbon powder. The porous carbon material electrodes with the “porous core structure” behaved superiorly at a specific capacitance of 320 F g^?1 at a current density of 0.05 A g^?1 in 6 M KOH electrolyte, which could still remain 193 F g^?1 when the current density increased to 100 A g^?1. Remarkably, in the 1 M TEABF₄/PC electrolyte, the PCM samples could reach 156 F g^?1 at 0.05 A g^?1, possess an outstanding energy density of 39.50 Wh kg^?1, and maintain at 22.05 Wh kg^?1 even when the power density rose up to 5880 W kg^?1. The balance of structural characteristic and high performance makes the porous carbon microbeads a competitive and promising supercapacitor electrode material.     

Porous Nitrogen‐Doped Carbon Microspheres Derived from Microporous Polymeric Organic Frameworks for High Performance Electric Double‐Layer Capacitors

This research presents a simple and efficient method to synthesize porous nitrogen‐doped carbon microspheres (PNCM) by the carbonization of microporous poly(terephthalaldehyde‐pyrrole) organic frameworks (PtpOF). The common KOH activation process is used to tune the porous texture of the PNCM and produce an activated‐PNCM (A‐PNCM). The PNCM and A‐PNCM with specific surface area of 921 and 1303 m² g^?1, respectively, are demonstrated as promising candidates for EDLCs. At a current density of 0.5 A g^?1, the specific capacitances of the PNCM and A‐PNCM are 248 and 282 F g^?1, respectively. At the relatively high current density of 20 A g^?1, the capacitance remaining is 95 and 154 F g^?1, respectively. Capacity retention of the A‐PNCM is more than 92 % after 10 000 charge/discharge cycles at a current density of 2 A g^?1.     

High‐Loading Nano‐SnO2 Encapsulated in situ in Three‐Dimensional Rigid Porous Carbon for Superior Lithium‐Ion Batteries

Tin oxide nanoparticles (SnO₂ NPs) have been encapsulated in situ in a three‐dimensional ordered space structure. Within this composite, ordered mesoporous carbon (OMC) acts as a carbon framework showing a desirable ordered mesoporous structure with an average pore size (≈6 nm) and a high surface area (470.3 m² g^?1), and the SnO₂ NPs (≈10 nm) are highly loaded (up to 80 wt %) and homogeneously distributed within the OMC matrix. As an anode material for lithium‐ion batteries, a SnO₂@OMC composite material can deliver an initial charge capacity of 943 mAh g^?1 and retain 68.9 % of the initial capacity after 50 cycles at a current density of 50 mA g^?1, even exhibit a capacity of 503 mA h g^?1 after 100 cycles at 160 mA g^?1. In situ encapsulation of the SnO₂ NPs within an OMC framework contributes to a higher capacity and a better cycling stability and rate capability in comparison with bare OMC and OMC ex situ loaded with SnO₂ particles (SnO₂/OMC). The significantly improved electrochemical performance of the SnO₂@OMC composite can be attributed to the multifunctional OMC matrix, which can facilitate electrolyte infiltration, accelerate charge transfer, and lithium‐ion diffusion, and act as a favorable buffer to release reaction strains for lithiation/delithiation of the SnO₂ NPs.     

Nitrogen‐Doped Carbon Monolith for Alkaline Supercapacitors and Understanding Nitrogen‐Induced Redox Transitions

A nitrogen‐doped porous carbon monolith was synthesized as a pseudo‐capacitive electrode for use in alkaline supercapacitors. Ammonia‐assisted carbonization was used to dope the surface with nitrogen heteroatoms in a way that replaced carbon atoms but kept the oxygen content constant. Ammonia treatment expanded the micropore size‐distributions and increased the specific surface area from 383 m² g^?1 to 679 m² g^?1. The nitrogen‐containing porous carbon material showed a higher capacitance (246 F g^?1) in comparison with the nitrogen‐free one (186 F g^?1). Ex situ electrochemical spectroscopy was used to investigate the evolution of the nitrogen‐containing functional groups on the surface of the N‐doped carbon electrodes in a three‐electrode cell. In addition, first‐principles calculations were explored regarding the electronic structures of different nitrogen groups to determine their relative redox potentials. We proposed possible redox reaction pathways based on the calculated redox affinity of different groups and surface analysis, which involved the reversible attachment/detachment of hydroxy groups between pyridone and pyridine. The oxidation of nitrogen atoms in pyridine was also suggested as a possible reaction pathway.     

Facile Synthesis of Nitrogen‐Containing Mesoporous Carbon for High‐Performance Energy Storage Applications

Porous carbon with high specific surface area (SSA), a reasonable pore size distribution, and modified surface chemistry is highly desirable for application in energy storage devices. Herein, we report the synthesis of nitrogen‐containing mesoporous carbon with high SSA (1390 m² g^?1), a suitable pore size distribution (1.5–8.1 nm), and a nitrogen content of 4.7 wt % through a facile one‐step self‐assembly process. Owing to its unique physical characteristics and nitrogen doping, this material demonstrates great promise for application in both supercapacitors and encapsulating sulfur as a superior cathode material for lithium–sulfur batteries. When deployed as a supercapacitor electrode, it exhibited a high specific capacitance of 238.4 F g^?1 at 1 A g^?1 and an excellent rate capability (180 F g^?1, 10 A g^?1). Furthermore, when an NMC/S electrode was evaluated as the cathode material for lithium–sulfur batteries, it showed a high initial discharge capacity of 1143.6 mA h g^?1 at 837.5 mA g^?1 and an extraordinary cycling stability with 70.3 % capacity retention after 100 cycles.     

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.     

Activated carbon prepared from polyaniline base by K2CO3 activation for application in supercapacitor electrodes

An activated carbon was prepared from a polyaniline base using K₂CO₃ as an activating agent. The morphology, surface chemical composition, and surface area of the as-prepared carbon materials were investigated by scanning electron microscope, X-ray photoelectron spectroscopy, and Brunauer?CEmmett?CTeller measurement, respectively. Electrochemical properties of the as-prepared sample were studied by cyclic voltammetry, galvanostatic charge/discharge, and electrochemical impedance spectroscopy measurements in 6?mol?L^?1 KOH aqueous solution. Compared with the non-activated carbon, activated carbon showed superior capacitive performance. The activation carbon presented a high specific gravimetric capacitance of 210?F?g^?1. The good electrochemical performance of the activated carbon was ascribed to well-developed micropores, high surface area, the presence of nitrogen and oxygen functional groups, and larger pore volume.     

Highly Ordered Mesoporous Few‐Layer Graphene Frameworks Enabled by Fe3O4 Nanocrystal Superlattices

While great progress has been achieved in the synthesis of ordered mesoporous carbons in the past decade, it still remains a challenge to prepare highly graphitic frameworks with ordered mesoporosity and high surface area. Reported herein is a simple synthetic methodology, based on the conversion of self‐assembled superlattices of Fe₃O₄ nanocrystals, to fabricate highly ordered mesoporous graphene frameworks (MGFs) with ultrathin pore walls consisting of three to six stacking graphene layers. The MGFs possess face‐centered‐cubic symmetry with interconnected mesoporosity, tunable pore width, and high surface area. Because of their unique architectures and superior structural durability, the MGFs exhibit excellent cycling stability and rate performance when used as anode materials for lithium‐ion batteries, thus retaining a specific capacity of 520 mAh g^?1 at a current density of 300 mA g^?1 after 400 cycles.     

Activated nitrogen-doped carbons from polyvinyl chloride for high-performance electrochemical capacitors

Activated nitrogen-doped carbons (ANCs) were prepared by carbonization/activation approach using aminated polyvinyl chloride (PVC) as precursor. ANCs exhibit larger porosities and higher specific surface areas than those of their nitrogen-free counterparts for the same KOH/carbon ratio. The specific surface area of ANC-1 is up to 1,398 m² g^?1 even at a low KOH/carbon ratio of 1:1. Fourier transform infrared spectroscopy investigation of the nitrogen-enriched resin precursor indicates the efficient dehydrochlorination of PVC by ethylenediamine at a low temperature. The nitrogen content and the population of nitrogen functionalities strongly depend on the KOH/carbon ratios and decrease drastically after KOH activation as seen from the elemental and X-ray photoelectron spectroscopy analysis. The surface concentration of N-6 and N-Q almost disappears and the dominant nitrogen groups become N-5 after KOH activation. The highest specific capacitance of ANCs is up to 345 F g^?1 at a current density of 50 mA g^?1 in 6 M KOH electrolyte. ANCs also exhibit a good capacitive behavior at a high scan rate of 200 mV s^?1 and an excellent cyclability with a capacitance retention ratio as high as ～93 % at a current density of 2,000 mA g^?1 for 5,000 cycles.     

Preparation of activated carbon from waste Camellia oleifera shell for supercapacitor application

The cost-effective activated carbons derived from waste Camellia oleifera shell (COS) by ZnCl₂ activation method are investigated as the active electrode material in electric double-layer capacitors (EDLCs) for the first time. The activation temperature and ZnCl₂/COS impregnation ratio are two key factors affecting the surface area and pore structure of the prepared activated carbons, which accordingly affect their capacitive performances. Electrochemical investigations indicate that the activated carbon (AC-3-600) obtained at the activation temperature of 600 °C and impregnation ratio of 3 shows the maximum specific capacitance of 374 and 266 F?g^?1 in 1 mol L^?1 H₂SO₄ and 6 mol L^?1 KOH electrolytes at 0.2 A g^?1, respectively. The high capacitance of the AC-3-600 is attributed to its high surface area (1,935 m² g^?1), high total pore volume (1.02 cm³ g^?1), and especially the large percentage of micropores (735 m² g^?1). Meanwhile, the activated carbon presents good cycle stability in both acid and alkaline electrolytes during 5,000 cycles at a fair current density of 4 A g^?1. So, we had reasons to believe that the activated carbons from waste COS by ZnCl₂ activation might be one of the innovative carbon electrode materials for EDLCs application.     

Hierarchical mesoporous carbon materials: preparation by direct tri-constituent co-assembly and the electrochemical performance

Hierarchical mesoporous carbon materials with large microporosity were prepared by direct tri-constituent co-assembly with the use of resols as the carbon precursor, tetraethyl orthosilicate as the inorganic precursor, and triblock copolymer F127 as the soft template. Bimodal pore size distributions in the range of 1.5–4 and 7.5–12 nm were obtained in the synthesized hierarchical mesoporous carbon materials after etching of silica by HF acid, showing a high surface area of 1,675 m²?g^?1 with a large pore volume of 2.06 cm³?g^?1. The electrochemical performance of the hierarchical mesoporous carbons was evaluated as an electrode material for electrochemical supercapacitor, showing a specific capacitance as high as 152 F?g^?1 at a scan rate of 5 mV?s^?1 in 6 M KOH aqueous solution and a good cycling stability with capacitance retention of 99 % over 500 cycles.     

MnO2 Nanosheets Grown on Nitrogen‐Doped Hollow Carbon Shells as a High‐Performance Electrode for Asymmetric Supercapacitors

A hierarchical hollow hybrid composite, namely, MnO₂ nanosheets grown on nitrogen‐doped hollow carbon shells (NHCSs@MnO₂), was synthesized by a facile in situ growth process followed by calcination. The composite has a high surface area (251 m²g^?1) and mesopores (4.5 nm in diameter), which can efficiently facilitate transport during electrochemical cycling. Owing to the synergistic effect of NHCSs and MnO₂, the composite shows a high specific capacitance of 306 F g^?1, good rate capability, and an excellent cycling stability of 95.2 % after 5000 cycles at a high current density of 8 A g^?1. More importantly, an asymmetric supercapacitor (ASC) assembled by using NHCSs@MnO₂ and activated carbon as the positive and negative electrodes exhibits high specific capacitance (105.5 F g^?1 at 0.5 A g^?1 and 78.5 F g^?1 at 10 A g^?1) with excellent rate capability, achieves a maximum energy density of 43.9 Wh kg^?1 at a power density of 408 W kg^?1, and has high stability, whereby the ASC retains 81.4 % of its initial capacitance at a current density of 5 A g^?1 after 4000 cycles. Therefore, the NHCSs@MnO₂ electrode material is a promising candidate for future energy‐storage systems.