Biomass Organs Control the Porosity of Their Pyrolyzed Carbon

In most electrochemical energy storage and conversion devices, nanostructured carbon materials play essential roles. One‐step carbonization of some biomass materials has recently been demonstrated as a promising route to produce high surface area carbon without introducing extra activation agents. Here, this study shows the importance of physiologic function of plant organs in the microstructure and porosity of formed carbon nanomaterials. The lotus stem pyrolyzed carbon at 800 °C presents a specific surface area of 1610 m² g^?1, about 55% higher than the porous carbon from the leaves. A similar organ‐dependent effect in the porosity of the pyrolyzed carbon is also observed in other plants with wide disparity in the stems and leaves, such as celery and asparagus lettuce, largely due to the higher metal ion content in the stems, which plays the role of ion transportation for plants. Furthermore, optimizing the celery stem pyrolyzing condition can produce carbon with specific surface area as high as 2194 m² g^?1 without any extra activation process. As a supercapacitor electrode, the porous carbon pyrolyzed from lotus stems exhibits a specific capacitance of 174 F g^?1 at a scan rate of 5 mV s^?1 in 6 M KOH aqueous electrolyte, with 72% capacitance retention at a high scan rate of 500 mV s^?1 and good stability over 10 000 cycles.     

Multifunctional Carbon for Electrochemical Double‐Layer Capacitors

Multifunctional carbon materials are prepared for application as an active electrode material in an electrochemical capacitor displaying both charge storage and binder properties. The synthesis of the materials involves the functionalization of high surface area Black Pearls 2000 carbon black by a covalent attachment of polyacrylic acid. The polyacrylic acid polymer is formed by atom transfer radical polymerization using 1‐(bromoethyl)benzene groups initially bonded to the carbon by spontaneous grafting from the corresponding diazonium ions. The grafting of 1‐(bromoethyl)benzene and polyacrylic acid is confirmed by thermogravimetric analysis, Fourier transform infrared spectroscopy, energy‐dispersive X‐ray spectroscopy, and nitrogen gas adsorption isotherm. The composite electrode films prepared from the modified carbon are more hydrophilic and have better wettability in an aqueous electrolyte than the one prepared with the unmodified carbon. The modified electrodes also show a higher specific capacitance (≈140 F g^?1), a wider working potential window (1.5 V) and excellent specific capacitance retention upon cycling (99.9% after 5000 cycles) in an aqueous 0.65 m K₂SO₄ electrolyte. Moreover, a relatively high specific capacitance (≈90 F g^?1) is maintained at a scan rate of 1000 mV s^?1 with the polyacrylic‐acid‐modified carbon electrode.     

Three‐Dimensional Co3O4@MnO2 Hierarchical Nanoneedle Arrays: Morphology Control and Electrochemical Energy Storage

In this paper, a highly ordered three‐dimensional Co₃O₄@MnO₂ hierarchical porous nanoneedle array on nickel foam is fabricated by a facile, stepwise hydrothermal approach. The morphologies evolution of Co₃O₄ and Co₃O₄@MnO₂ nanostructures upon reaction times and growth temperature are investigated in detail. Moreover, the as‐prepared Co₃O₄@MnO₂ hierarchical structures are investigated as anodes for both supercapacitors and Li‐ion batteries. When used for supercapacitors, excellent electrochemical performances such as high specific capacitances of 932.8 F g^?1 at a scan rate of 10 mV s^?1 and 1693.2 F g^?1 at a current density of 1 A g^?1 as well as long‐term cycling stability and high energy density (66.2 W h kg^?1 at a power density of 0.25 kW kg^?1), which are better than that of the individual component of Co₃O₄ nanoneedles and MnO₂ nanosheets, are obtained. The Co₃O₄@MnO₂ NAs are also tested as anode material for LIBs for the first time, which presents an improved performance with high reversible capacity of 1060 mA h g^?1 at a rate of 120 mA g^?1, good cycling stability, and rate capability.     

Ultrahigh‐Performance Pseudocapacitor Electrodes Based on Transition Metal Phosphide Nanosheets Array via Phosphorization: A General and Effective Approach

In this study, a general and effective phosphorization strategy is successfully demonstrated to enhance supercapacitor performance of various transition metals oxide or hydroxide, such as Ni(OH)₂, Co(OH)₂, MnO₂, and Fe₂O₃. For example, a 3D networked Ni₂P nanosheets array via a facile phosphorization reaction of Ni(OH)₂ nanosheets is grown on the surface of a Ni foam. The Ni foam‐supported Ni₂P nanosheet (Ni₂P NS/NF) electrode shows a remarkable specific capacitance of 2141 F g^?1 at a scan rate of 50 mV s^?1 and remains as high as 1109 F g^?1 even at the current density of 83.3 A g^?1. The specific capacitance is much larger than those of Ni(OH)₂ NS/NF (747 F g^?1 at 50 mV s^?1). Furthermore, the electrode retains a high specific capacitance of 1437 F g^?1 even after 5000 cycles at a current density of 10 A g^?1, in sharp contrast with only 403 F g^?1 of Ni(OH)₂ NS/NF at the same current density. The similar enhanced performance is observed for Ni₂P powder, which eliminates the influence of nickel foam. The enhanced supercapacitor performances are attributed to the 3D porous nanosheets network, enhanced conductivity, and two active components of Ni²⁺ and P^δ? with rich valences of Ni₂P.     

Breaking the Limits of Ionic Liquid‐Based Supercapacitors: Mesoporous Carbon Electrodes Functionalized with Manganese Oxide Nanosplotches for Dense,Stable, and Wide‐Temperature Energy Storage

Manganese oxide (MnO₂) nanosplotches (NSs) are deposited on N‐ and S‐doped ordered mesoporous carbon (N,S‐CMK‐3) essentially blocking microporosity. The obtained N,S‐CMK‐3/MnO₂ composite materials are assembled into ionic liquid (IL)‐based symmetric supercapacitors, which exhibit a high specific capacitance of 200 F g^?1 (0–3.5 V) at a scan rate of 2 mV s^?1, and good rate stability with 55.5% capacitance retention at a scan rate of 100 mV s^?1. The device can operate in a wide temperature range (?20 to 60 °C), and high cycling stability of N,S‐CMK‐3/MnO₂ composite electrode is demonstrated. Lower energy of ?3.56 eV can be achieved for the adsorption of 1‐ethyl‐3‐methylimidazolium⁺ (EMIM⁺) cation on the edge between MnO₂ NSs and N,S‐CMK‐3 than on the plane of MnO₂ NS (?3.04 eV), both being more preferred than the surface of pristine N,S‐CMK‐3 (?1.52 eV). This strengthening of the ion adsorption at the three‐phase boundary between N,S‐CMK‐3, MnO₂, and IL leads to enhancement of the specific capacity as compared to nondoped or MnO₂‐free reference materials. Supercapacitors based on such composite electrodes show significantly enhanced areal capacity pointing to energy storage in the mesopores rather than in the electrochemical surface layer, demonstrating a new energy storage mechanism in ILs.     

Boosting the Electrical Double‐Layer Capacitance of Graphene by Self‐Doped Defects through Ball‐Milling

Improving the capacitance of carbon materials for supercapacitors without sacrificing their rate performance, especially volumetric capacitance at high mass loadings, is a big challenge because of the limited assessable surface area and sluggish electrochemical kinetics of the pseudocapacitive reactions. Here, it is demonstrated that “self‐doping” defects in carbon materials can contribute to additional capacitance with an electrical double‐layer behavior, thus promoting a significant increase in the specific capacitance. As an exemplification, a novel defect‐enriched graphene block with a low specific surface area of 29.7 m² g^?1 and high packing density of 0.917 g cm^?3 performs high gravimetric, volumetric, and areal capacitances of 235 F g^?1, 215 F cm^?3, and 3.95 F cm^?2 (mass loading of 22 mg cm^?2) at 1 A g^?1, respectively, as well as outstanding rate performance. The resulting specific areal capacitance reaches an ultrahigh value of 7.91 F m^?2 including a “self‐doping” defect contribution of 4.81 F m^?2, which is dramatically higher than the theoretical capacitance of graphene (0.21 F m^?2) and most of the reported carbon‐based materials. Therefore, the defect engineering route broadens the avenue to further improve the capacitive performance of carbon materials, especially for compact energy storage under limited surface areas.     

Layered Silicon‐Based Nanosheets as Electrode for 4 V High‐Performance Supercapacitor

Silicon‐based materials have shown great potential and been widely studied in various fields. Unlike its unparalleled theoretical capacity as anodes for batteries, few investigations have been reported on silicon‐based materials for applications in supercapacitors. Here, an electrode composed of layered silicon‐based nanosheets, obtained through oxidation and exfoliation, for a supercapacitor operated up to 4 V is reported. These silicon‐based nanosheets show an areal specific capacitance of 4.43 mF cm^?2 at 10 mV s^?1 while still retaining a specific capacitance of 834 µF cm^?2 even at an ultrahigh scan rate of 50 000 mV s^?1. The volumetric energy and power density of the supercapacitor are 7.65 mWh cm^?3 and 9312 mW cm^?3, respectively, and the electrode can operate for 12000 cycles in a potential window of 4 V at 2 A g^?1, while retaining 90.6% capacitance. These results indicate that the silicon‐based nanosheets can be a competitive candidate as the supercapacitor electrode material.     

Ultralight and Binder‐Free All‐Solid‐State Flexible Supercapacitors for Powering Wearable Strain Sensors

Flexible energy storage devices play a pivotal role in realizing the full potential of flexible electronics. This work presents high‐performance, all‐solid‐state, flexible supercapacitors by employing an innovative multilevel porous graphite foam (MPG). MPGs exhibit superior properties, such as large specific surface area, high electric conductivity, low mass density, high loading efficiency of pseudocapacitive materials, and controlled corrugations for accommodating mechanical strains. When loaded with pseudocapacitive manganese oxide (Mn₃O₄), the MPG/Mn₃O₄ (MPGM) composites achieve a specific capacitance of 538 F g^?1 (1 mV s^?1) and 260 F g^?1 (1 mV s^?1) based on the mass of pure Mn₃O₄ and entire electrode composite, respectively. Both are among the best of Mn₃O₄‐based supercapacitors. The MPGM is mechanically robust and can go through 1000 mechanical bending cycles with only 1.5% change in electric resistance. When integrated as all‐solid‐state symmetric supercapacitors, they offer a full cell specific capacitance as high as 53 F g^?1 based on the entire electrode and retain 80% of capacitance after 1000 continuous mechanical bending cycles. Furthermore, the all‐solid‐state flexible supercapacitors are incorporated with strain sensors into self‐powered flexible devices for detection of both coarse and fine motions on human skins, i.e., those from finger bending and heart beating.     

Dual Support System Ensuring Porous Co–Al Hydroxide Nanosheets with Ultrahigh Rate Performance and High Energy Density for Supercapacitors

Layered double hydroxides (LDHs) are promising supercapacitor electrode materials due to their high specific capacitances. However, their electrochemical performances such as rate performance and energy density at a high current density, are rather poor. Accordingly, a facile strategy is demonstrated for the synthesis of the integrated porous Co–Al hydroxide nanosheets (named as GSP‐LDH) with dual support system using dodecyl sulfate anions and graphene sheets as structural and conductive supports, respectively. Owing to fast ion/electron transport, porous and integrated structure, the GSP‐LDH electrode exhibits remarkably improved electrochemical characteristics such as high specific capacitance (1043 F g^?1 at 1 A g^?1) and ultra‐high rate performance capability (912 F g^?1 at 20 A g^?1). Moreover, the assembled sandwiched graphene/porous carbon (SGC)//GSP‐LDH asymmetric supercapacitor delivers a high energy density up to 20.4 Wh kg^?1 at a very high power density of 9.3 kW kg^?1, higher than those of previously reported asymmetric supercapacitors. The strategy provides a facile and effective method to achieve high rate performance LDH based electrode materials for supercapacitors.     

Ultrathin Mesoporous NiCo2O4 Nanosheets Supported on Ni Foam as Advanced Electrodes for Supercapacitors

A facile two‐step method is developed for large‐scale growth of ultrathin mesoporous nickel cobaltite (NiCo₂O₄) nanosheets on conductive nickel foam with robust adhesion as a high‐performance electrode for electrochemical capacitors. The synthesis involves the co‐electrodeposition of a bimetallic (Ni, Co) hydroxide precursor on a Ni foam support and subsequent thermal transformation to spinel mesoporous NiCo₂O₄. The as‐prepared ultrathin NiCo₂O₄ nanosheets with the thickness of a few nanometers possess many interparticle mesopores with a size range from 2 to 5 nm. The nickel foam supported ultrathin mesoporous NiCo₂O₄ nanosheets promise fast electron and ion transport, large electroactive surface area, and excellent structural stability. As a result, superior pseudocapacitive performance is achieved with an ultrahigh specific capacitance of 1450 F g^?1, even at a very high current density of 20 A g^?1, and excellent cycling performance at high rates, suggesting its promising application as an efficient electrode for electrochemical capacitors.     

Ternary Hybrids of Amorphous Nickel Hydroxide–Carbon Nanotube‐Conducting Polymer for Supercapacitors with High Energy Density,Excellent Rate Capability,and Long Cycle Life

The utilization of Ni(OH)₂ as a pseudocapacitive material for high performance supercapacitors is hindered by its low electrical conductivity and short cycle life. A coaxial ternary hybrid material comprising of amorphous Ni(OH)₂ deposited on multiwalled carbon nanotubes wrapped with conductive polymer (poly (3,4‐ethylenedioxythiophene)‐poly(styrenesulfonate)) is demonstrated. A thin layer of disordered amorphous Ni(OH)₂ is deposited by an effective “coordinating etching and precipitating” method, resulting in an ultrahigh specific capacitance of 3262 F g^?1 at 5 mV s^?1 and excellent rate capability (71.9% capacitance retention at 100 mV s^?1). More importantly, the polymer layer prevents the degradation of the nanostructure and dis­solution of Ni ion during repeated charge–discharge cycling for 30 000 cycles, a phenomenon which often plagues Ni(OH)₂ nanomaterials. Using the ternary Ni(OH)₂ hybrid and the reduced graphene oxide/carbon nanotube hybrid as the positive and negative electrodes, respectively, the assembled asymmetric supercapacitors exhibit high energy density of 58.5 W h kg^?1 at the power density of 780 W kg^?1 as well as long cycle life (86% capacitance retention after 30 000 cycles). The ternary hybrid architecture design for amorphous Ni(OH)₂ can be regarded as a general approach to obtain pseudocapacitive materials for supercapacitors with both high energy density, excellent rate capability, and long cycle life.     

Design of Hierarchical NiCo@NiCo Layered Double Hydroxide Core–Shell Structured Nanotube Array for High‐Performance Flexible All‐Solid‐State Battery‐Type Supercapacitors

A novel hierarchical nanotube array (NTA) with a massive layered top and discretely separated nanotubes in a core–shell structure, that is, nickel–cobalt metallic core and nickel–cobalt layered double hydroxide shell (Ni?Co@Ni?Co LDH), is grown on carbon fiber cloth (CFC) by template‐assisted electrodeposition for high‐performance supercapacitor application. The synthesized Ni?Co@Ni?Co LDH NTAs/CFC shows high capacitance of 2200 F g^?1 at a current density of 5 A g^?1, while 98.8% of its initial capacitance is retained after 5000 cycles. When the current density is increased from 1 to 20 A g^?1, the capacitance loss is less than 20%, demonstrating excellent rate capability. A highly flexible all‐solid‐state battery‐type supercapacitor is successfully fabricated with Ni?Co LDH NTAs/CFC as the positive electrode and electrospun carbon fibers/CFC as the negative electrode, showing a maximum specific capacitance of 319 F g^?1, a high energy density of 100 W h kg^?1 at 1.5 kW kg^?1, and good cycling stability (98.6% after 3000 cycles). These fascinating electrochemical properties are resulted from the novel structure of electrode materials and synergistic contributions from the two electrodes, showing great potential for energy storage applications.     

Design of Hierarchical Ni?Co@Ni?Co Layered Double Hydroxide Core–Shell Structured Nanotube Array for High‐Performance Flexible All‐Solid‐State Battery‐Type Supercapacitors

A novel hierarchical nanotube array (NTA) with a massive layered top and discretely separated nanotubes in a core–shell structure, that is, nickel–cobalt metallic core and nickel–cobalt layered double hydroxide shell (Ni? Co@Ni? Co LDH), is grown on carbon fiber cloth (CFC) by template‐assisted electrodeposition for high‐performance supercapacitor application. The synthesized Ni? Co@Ni? Co LDH NTAs/CFC shows high capacitance of 2200 F g^?1 at a current density of 5 A g^?1, while 98.8% of its initial capacitance is retained after 5000 cycles. When the current density is increased from 1 to 20 A g^?1, the capacitance loss is less than 20%, demonstrating excellent rate capability. A highly flexible all‐solid‐state battery‐type supercapacitor is successfully fabricated with Ni? Co LDH NTAs/CFC as the positive electrode and electrospun carbon fibers/CFC as the negative electrode, showing a maximum specific capacitance of 319 F g^?1, a high energy density of 100 W h kg^?1 at 1.5 kW kg^?1, and good cycling stability (98.6% after 3000 cycles). These fascinating electrochemical properties are resulted from the novel structure of electrode materials and synergistic contributions from the two electrodes, showing great potential for energy storage applications.     

A Dendritic Nickel Cobalt Sulfide Nanostructure for Alkaline Battery Electrodes

A uniform dendritic NiCo₂S₄@NiCo₂S₄ hierarchical nanostructure of width ≈100 nm is successfully designed and synthesized. From kinetic analysis of the electrochemical reactions, those electrodes function in rechargeable alkaline batteries (RABs). The dendritic structure exhibited by the electrodes has a high discharge‐specific capacity of 4.43 mAh cm^?2 at a high current density of 240 mA cm^?2 with a good rate capability of 70.1% after increasing the current densities from 40 to 240 mA cm^?2. At low scan rate of 0.5 mV s^?1 in cyclic voltammetry test, the semidiffusion controlled electrochemical reaction contributes ≈92% of the total capacity, this value decreases to ≈43% at a high scan rate of 20 mV s^?1. These results enable a detailed analysis of the reaction mechanism for RABs and suggest design concepts for new electrode materials.     

Multilayer‐Folded Graphene Ribbon Film with Ultrahigh Areal Capacitance and High Rate Performance for Compressible Supercapacitors

Limited by 2D geometric morphology and low bulk packing density, developing graphene‐based flexible/compressible supercapacitors with high specific capacitances (gravimetric/volumetric/areal), especially at high rates, is an outstanding challenge. Here, a strategy for the synthesis of free‐standing graphene ribbon films (GRFs) for high‐performance flexible and compressible supercapacitors through blade‐coating of interconnected graphene oxide ribbons and a subsequent thermal treatment process is reported. With an ultrahigh mass loading of 21 mg cm^?2, large ion‐accessible surface area, efficient electron and ion transport pathways as well as high packing density, the compressed multilayer‐folded GRF films (F‐GRF) exhibit ultrahigh areal capacitance of 6.7 F cm^?2 at 5 mA cm^?2, high gravimetric/volumetric capacitances (318 F g^?1, 293 F cm^?3), and high rate performance (3.9 F cm^?2 at 105 mA cm^?2), as well as excellent cycling stability (109% of capacitance retention after 40 000 cycles). Furthermore, the assembled F‐GRF symmetric supercapacitor with compressible and flexible characteristics, can deliver an ultrahigh areal energy density of 0.52 mWh cm^?2 in aqueous electrolyte, almost two times higher than the values obtained from symmetric supercapacitors with comparable dimensions.     

ZnO Hard Templating for Synthesis of Hierarchical Porous Carbons with Tailored Porosity and High Performance in Lithium‐Sulfur Battery

Hierarchical porous carbon (HPC, DUT‐106) with tailored pore structure is synthesized using a versatile approach based on ZnO nanoparticles avoiding limitations present in conventional silica hard templating approaches. The benefit of the process presented here is the removal of all pore building components by pyrolysis of the ZnO/carbon composite without any need for either toxic/reactive gases or purification of the as‐prepared hierarchical porous carbon. The carbothermal reduction process is accompanied by an advantageous growing of distinctive micropores within the thin carbon walls. The resulting materials show not only high internal porosity (total pore volume up to 3.9 cm³ g^?1) but also a large number of electrochemical reaction sites due to their remarkably high specific surface area (up to 3060 m² g^?1), which renders them particularly suitable for the application as sulfur host material. Applied in the lithium‐sulfur battery, the HPC/sulfur composite exhibits a capacity of >1200 mAh g^?1‐sulfur (>750 mAh g^?1 electrode) at a high sulfur loading of ≥ 3 mg cm^?2 as well as outstanding rate capability. In fact, this impressive performance is achieved even using a low amount of electrolyte (6.8 μl mg^?1 _sulfur) allowing for further weight reduction and maintenance of high energy density on cell level.     

Block‐Copolymer‐Templated Synthesis of Electroactive RuO2‐Based Mesoporous Thin Films

RuO₂‐based mesoporous thin films of optical quality are synthesized from ruthenium‐peroxo‐based sols using micelle templates made of amphiphilic polystyrene‐polyethylene oxide block copolymers. The mesoporous structure and physical properties of the RuO₂ films (mesoporous volume: 30%; pore diameter: ～30 nm) can be controlled by the careful tuning of both the precursor solution and thermal treatment (150–350 °C). The optimal temperature that allows control of both mesoporosity and nanocristallinity is strongly dependent on the substrate (silicon or fluorine‐doped tin oxide). The structure of the resulting mesoporous films are investigated using X‐ray diffraction, X‐ray photoelectron spectroscopy, and atomic force microscopy. Mesoporous layers are additionally characterized by transmission and scanning electron microscopy and ellipsometry while their electrochemical properties are analyzed via cyclic voltammetry. Thick mesoporous films of ruthenium oxide hydrates, RuO₂ · xH₂O, obtained using a thermal treatment at 280 °C, exhibit capacitances as high as 1000 ± 100 F g^?1 at a scan rate of 10 mV s^?1, indicating their potential application as electrode materials.     

Necklace‐like Nitrogen‐Doped Tubular Carbon 3D Frameworks for Electrochemical Energy Storage

The design and synthesis of a necklace‐like nitrogen‐doped tubular carbon (NTC) are presented by growing microporous polyhedral ZIF‐8 particles and a uniform layer of ZIF‐8 on sacrificial ZnO tetrapods (ZTPs). Oxygen vacancies together with defect regions on the surface of the ZTPs result in the formation of ZIF‐8 polyhedra in conjunction with a very thin shell. This necklace‐like NTC structure has a high N content, very large surface area, ultrahigh microporosity, and quite high electrical conductivity. NTC‐based symmetrical supercapacitor and zinc‐ion capacitor (ZIC) devices are fabricated and their electrochemical performance is measured. The NTC supercapacitor shows an ultrahigh rate capability (up to 2000 mV s^?1) and promising cycle life, retaining 91.5% of its initial performance after 50 000 galvanostatic charge–discharge cycles. An aqueous ZIC, constructed using the NTC, has a specific capacitance of 341.2 F g^?1 at a current density of 0.1 A g^?1 and an energy density of 189.6 Wh kg^?1 with a 2.0‐V voltage window, respectively. The outstanding performance is attributed to the NTC high N‐doping content, a continuous “polyhedral 3D hollow” architecture and the highly porous microtubular arms exhibiting very high surface area.     

Prolifera‐Green‐Tide as Sustainable Source for Carbonaceous Aerogels with Hierarchical Pore to Achieve Multiple Energy Storage

The increasing demand for efficient energy storage and conversion devices has aroused great interest in designing advanced materials with high specific surface areas, multiple holes, and good conductivity. Here, we report a new method for fabricating a hierarchical porous carbonaceous aerogel (HPCA) from renewable seaweed aerogel. The HPCA possesses high specific surface area of 2200 m² g^?1 and multilevel micro/meso/macropore structures. These important features make HPCA exhibit a reversible lithium storage capacity of 827.1 mAh g^?1 at the current density of 0.1 A g^?1, which is the highest capacity for all the previously reported nonheteroatom‐doped carbon nanomaterials. It also shows high specific capacitance and excellent rate performance for electric double layer capacitors (260.6 F g^?1 at 1 A g^?1 and 190.0 F g^?1 at 50 A g^?1), and long cycle life with 91.7% capacitance retention after 10 000 cycles at 10 A g^?1. The HPCA also can be used as support to assemble Co₃O₄ nanowires (Co₃O₄@HPCA) for constructing a high performance pseudocapacitor with the maximum specific capacitance of 1167.6 F g^?1 at the current density of 1 A g^?1. The present work highlights the first example in using prolifera‐green‐tide as a sustainable source for developing advanced carbon porous aerogels to achieve multiple energy storage.     

Micro‐Supercapacitors Based on Interdigital Electrodes of Reduced Graphene Oxide and Carbon Nanotube Composites with Ultrahigh Power Handling Performance

A novel method for fabricating micro‐patterned interdigitated electrodes based on reduced graphene oxide (rGO) and carbon nanotube (CNT) composites for ultra‐high power handling micro‐supercapacitor application is reported. The binder‐free microelectrodes were developed by combining electrostatic spray deposition (ESD) and photolithography lift‐off methods. Without typically used thermal or chemical reduction, GO sheets are readily reduced to rGO during the ESD deposition. Electrochemical measurements show that the in‐plane interdigital design of the microelectrodes is effective in increasing accessibility of electrolyte ions in‐between stacked rGO sheets through an electro‐activation process. Addition of CNTs results in reduced restacking of rGO sheets and improved energy and power density. Cyclic voltammetry (CV) measurements show that the specific capacitance of the micro‐supercapacitor based on rGO–CNT composites is 6.1 mF cm^?2 at 0.01 V s^?1. At a very high scan rate of 50 V s^?1, a specific capacitance of 2.8 mF cm^?2 (stack capacitance of 3.1 F cm^?3) is recorded, which is an unprecedented performance for supercapacitors. The addition of CNT, electrolyte‐accessible and binder‐free microelectrodes, as well as an interdigitated in‐plane design result in a high‐frequency response of the micro‐supercapacitors with resistive‐capacitive time constants as low as 4.8 ms. These characteristics suggest that interdigitated rGO–CNT composite electrodes are promising for on‐chip energy storage application with high power demands.