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1.
Manganese dioxide (MnO2) materials have received much attention as promising pseudocapacitive materials owing to their high theoretical capacitance and natural abundance. Unfortunately, the charge storage performance of MnO2 is usually limited to commercially available mass loading electrodes because of the significantly lower electron and ion migration kinetics in thick electrodes. Here, an alternatively assembled 2D layered material consisting of exfoliated MnO2 nanosheets and nitrogen-doped carbon layers for ultrahigh-mass-loading supercapacitors without sacrificing energy storage performance is reported. Layered birnessite-type MnO2 is efficiently exfoliated and intercalated by a carbon precursor of dopamine using a fluid dynamic-induced process, resulting in MnO2/nitrogen-doped carbon (MnO2/C) materials after self-polymerization and carbonization. The alternatively stacked and interlayer-expanded structure of MnO2/C enables fast and efficient electron and ion transfer in a thick electrode. The resulting MnO2/C electrode shows outstanding electrochemical performance at an ultrahigh mass loading of 19.7 mg cm−2, high gravimetric and areal capacitances of 480.3 F g−1 and 9.4 F cm−2 at 0.5 mA cm−2, and rapid charge/discharge capability of 70% capacitance retention at 40 mA cm−2. Furthermore, asymmetric supercapacitor based on high-mass-loading MnO2/C can deliver an extremely high energy of 64.2 Wh kg−1 at a power density of 18.8 W kg−1 in an aqueous electrolyte.  相似文献   

2.
The freestanding MXene films are promising for compact energy storage ascribing to their high pseudocapacitance and density, yet the sluggish ion transport caused by the most densely packed structure severely hinders their rate capability. Here, a reassembly strategy for constructing freestanding and flexible MXene-based film electrodes with a tunable porous structure is proposed, where the Ti3C2Tx microgels disassembled from 3D structured hydrogel are reassembled together with individual Ti3C2Tx nanosheets in different mass ratios to form a densely packed 3D network in microscale and a film morphology in macroscale. The space utilization of produced film can be maximized by a good balance of the density and porosity, resulting in a high volumetric capacitance of 736 F cm−3 at an ultrahigh scan rate of 2000 mV s−1. The fabricated supercapacitor yields a superior energy density of 40 Wh L−1 at a power density of 0.83 kW L−1, and an energy density of 21 Wh L−1 can be still maintained even when the power density reaches 41.5 kW L−1, which are the highest values reported to date for symmetric supercapacitors in aqueous electrolytes. More promisingly, the reassembled films can be used as electrodes of flexible supercapacitors, showing excellent flexibility and integrability.  相似文献   

3.
Although challenging, the fabricated supercapacitor electrodes with excellent rate capability, long cycling stability, and high mass-loading are crucial for practical applications. Herein, a novel 3D porous poly(p-aminoazobenzene)/reduced graphene oxide hydrogel is designed and prepared as an ultrafast, high-loading, and durable pseudocapacitive electrode through a facile two-step self-assembly approach. Owing to abundant stable redox-active sites, fast electrolyte diffusion, and efficient charge conduction, the PRH electrode (5 mg cm−2) shows a high specific capacitance (701 F g−1 at 2 A g−1) and ultrafast rate (97% capacitance retention at 100 A g−1). Furthermore, even with a mass-loading of 10 mg cm−2, the electrode still exhibits comparable high performance and excellent long-term cycling life (only 6.7% capacitance loss after 10 000 cycles). This work demonstrates novel polyaniline analog composites for constructing novel electrodes, promising to open an avenue toward practical applications.  相似文献   

4.
Flexible electrodes of ternary composites, in which highly conductive carbon nanotube films (CNFs) are coated with carbon nanotube-doped graphene oxide/polypyrrole (CNT-GO/PPy), have been fabricated via facile electrochemical synthesis. Long and short CNTs are separately doped into the composites (lCNT-GO/PPy and sCNT-GO/PPy) and their electrochemical performances are compared. Electrochemical measurements indicate that the doping of CNTs in the composites significantly improves the electrochemical behaviors of the GO/PPy electrodes. Notably, the lCNT-GO/PPy electrodes show superior electrochemical properties with respect to the sCNT-GO/PPy electrodes, which is related to the introduction of abundant CNTs in the former electrodes and their special microstructures. Two symmetric electrodes with the lCNT-GO/PPy composites coated on CNFs are assembled to fabricate a solid-state supercapacitor device, which features lightweight, ultrathinness, and high flexibility. The device achieves a high areal and volumetric specific capacitance of 70.0 mF cm−2 at 10 mV s−1 and 6.3 F cm−3 at 0.043 A cm−3, respectively. It also shows superior rate performance and cycle stability, with a capacitance retention rate of 87.7% for 10,000 cycles. The supercapacitor device fabricated is promising for the use in lightweight and flexible integrated electronics.  相似文献   

5.
The design of pseudocapacitive electrodes that exhibit high-rate and high volumetric capacitances is a big challenge, since it requires subtle modulation of ion-intercalation structures that are able to achieve high electrochemical activity, fast ion transport, and facilitated electron transfer, simultaneously. Herein, controllable and selective etching of B atoms from B-doped Ti3AlC2 precursors is reported, which generates boron-vacancy doped MXene (B-V-MXene) nanosheets with finely-regulated, ion-intercalation structures. Electrochemical studies and density-functional-theory calculations demonstrate that Ti around vacancies possess higher surface-redox activity with protons than those on pristine MXenes for the improvement of capacitances. In addition, interlayer spacing can be optimized on B-V-MXenes in promoting proton intercalation. More importantly, the dopant B atoms can increase the electron density on Ti, facilitating the adsorption of the intercalated protons; and further, B 2p-Ti 3d hybridized band sits closer to the Fermi energy than that of C 2p bands, which bridges the energy gap for electron transfer in the pseudo-capacitive reaction. With synergy of all these effects, the novel B-V-MXene compact electrodes can deliver the previously unmatched high volumetric capacitances of 807 F cm−3 at 1,000 mV s−1 and 1,815 F cm−3 at 5 mV s−1, with excellent cycle stability over 10,000 cycles.  相似文献   

6.
The development of flexible electrodes with high mass loading and efficient electron/ion transport is of great significance but still remains the challenge of innovating suitable electrode structures for high energy density application. Herein, for the first time, lignosulfonate-derived N/S-co-doped graphene-like carbon is in situ formed within an interface engineered cellulose textile through a sacrificial template method. Both experimental and theoretical calculations disclose that the formed pomegranate-like structure with continuous conductive pathways and porous characteristics allows sufficient ion/electron transport throughout the entire structures. As a result, the obtained flexible electrode delivers a remarkable integrated capacitance of 6534 mF cm−2 (335.1 F g−1) and a superior stability at an industrially applicable mass loading of 19.5 mg cm−2. A pseudocapacitive cathode with ultrahigh capacitance of 7000 mF cm−2 can also be obtained based on the same electrode structure engineering. The as-assembled asymmetric supercapacitor achieves a high areal capacitance of 3625 mF cm−2, and a maximum energy density of 1.06 mWh cm−2, outperforms most of other reported high-loading supercapacitors. This synthesis method and structural engineering strategy can provide materials design concepts and a wide range of applications in the fields of energy storage beyond supercapacitors.  相似文献   

7.
Designing energy storage devices from thick carbon electrodes with high areal/volumetric energy density via a simple and green way is very attractive but still challenging. Cellulose, as an excellent precursor for thick carbon electrodes with abundant sources and low cost, is usually activated by a chemical activator and pyrolysis route to achieve high electrochemical performance. However, there are still some problems to be addressed, such as the harsh activation conditions, easy collapse of porous structures, and the high cost. Herein, a 3D self-supporting thick carbon electrode derived from wood-based cellulose is proposed for high areal and volumetric energy density of supercapacitor from a mild, simple, and green enzymolysis treatment. Benefiting from the high specific surface area (1418 m2 g−1) and abundant active sites on the surface of wood-derived hierarchically porous structures and enzymolysis-induced micropores and mesopores, the assembled symmetry supercapacitor from the thick carbon electrode can realize the high areal/volumetric energy density of 0.21 mWh cm−2/0.99 mWh cm−3 with excellent stability of 86.58% after 15 000 long-term cycles at 20 mA cm−2. Significantly, the simple and universal strategy to design material with high specific surface area, provides a new research idea for realizing multi-functional application.  相似文献   

8.
A strategy to prepare flexible and conductive MXene/graphene (reduced graphene oxide, rGO) supercapacitor electrodes by using electrostatic self‐assembly between positively charged rGO modified with poly(diallyldimethylammonium chloride) and negatively charged titanium carbide MXene nanosheets is presented. After electrostatic assembly, rGO nanosheets are inserted in‐between MXene layers. As a result, the self‐restacking of MXene nanosheets is effectively prevented, leading to a considerably increased interlayer spacing. Accelerated diffusion of electrolyte ions enables more electroactive sites to become accessible. The freestanding MXene/rGO‐5 wt% electrode displays a volumetric capacitance of 1040 F cm?3 at a scan rate of 2 mV s?1 , an impressive rate capability with 61% capacitance retention at 1 V s?1 and long cycle life. Moreover, the fabricated binder‐free symmetric supercapacitor shows an ultrahigh volumetric energy density of 32.6 Wh L?1, which is among the highest values reported for carbon and MXene based materials in aqueous electrolytes. This work provides fundamental insight into the effect of interlayer spacing on the electrochemical performance of 2D hybrid materials and sheds light on the design of next‐generation flexible, portable and highly integrated supercapacitors with high volumetric and rate performances.  相似文献   

9.
The application of nontoxic 2D transition-metal carbides (MXenes) has recently gained ground in bioelectronics. In group-4 transition metals, tantalum possesses enhanced biological and physical properties compared to other MXene counterparts. However, the application of tantalum carbide for bioelectrodes has not yet been explored. Here, fluorine-free exfoliation and functionalization of tantalum carbide MAX-phase to synthesize a novel Ta4C3Tx MXene-tantalum oxide (TTO) hybrid structure through an innovative, facile, and inexpensive protocol is demonstrated. Additionally, the application of TTO composite as an efficient biocompatible material for supercapacitor electrodes is reported. The TTO electrode displays long-term stability over 10 000 cycles with capacitance retention of over 90% and volumetric capacitance of 447 F cm−3 (194 F g−1) at 1 mV s−1. Furthermore, TTO shows excellent biocompatibility with human-induced pluripotent stem cells-derived cardiomyocytes, neural progenitor cells, fibroblasts, and mesenchymal stem cells. More importantly, the electrochemical data show that TTO outperforms most of the previously reported biomaterials-based supercapacitors in terms of gravimetric/volumetric energy and power densities. Therefore, TTO hybrid structure may open a gateway as a bioelectrode material with high energy-storage performance for size-sensitive applications.  相似文献   

10.
2D MXene materials are of considerable interest for future energy storage. A MXene film could be used as an effective flexible supercapacitor electrode due to its flexibility and, more importantly, its high specific capacitance. However, although it has excellent electronic conductivity, sluggish ionic kinetics within the MXene film becomes a fundamental limitation to the electrochemical performance. To compensate for the relative deficiency, MXene films are frequently reduced to several micrometer dimensions with low mass loading (<1 mg cm?2), to the point of detriment of areal performance and commercial value. Herein, for the first time, the design of a 3D porous MXene/bacterial cellulose (BC) self‐supporting film is reported for ultrahigh capacitance performance (416 F g?1, 2084 mF cm?2) with outstanding mechanical properties and high flexibility, even when the MXene loading reaches 5 mg cm?2. The highly interconnected MXene/BC network enables both excellent electron and ion transport channel. Additionally, a maximum energy density of 252 µWh cm?2 is achieved in an asymmetric supercapacitor, higher than that of all ever‐reported MXene‐based supercapacitors. This work exploits a simple route for assembling 2D MXene materials into 3D porous films as state‐of‐the‐art electrodes for high performance energy storage devices.  相似文献   

11.
MXenes, 2D transition metal carbides, and nitrides have attracted tremendous interest because of their metallic conductivity, solution processability, and excellent merits in energy storage and other applications. However, the pristine MXene films often suffer from poor ambient stability and mechanical properties that stem from their polar terminal groups and weak interlayer interactions. Here, a heteroatom doping strategy is developed to tailor the surface functionalities of MXene, followed by the addition of large-sized reduced graphene oxide (rGO) as conductive additives to achieve a scalable production of S, N-MXene/rGO (SNMG-40) hybrid film with high mechanical strength ( ≈ 45 MPa) and energy storage properties (698.5 F cm−3). Notably, the SNMG-40 film also demonstrates long-term cycling stability ( ≈ 98% capacitance retention after 30 000 cycles), which can be maintained under ambient condition or immersed in H2SO4 electrolyte for more than 100 days. The asymmetric supercapacitor (aMGSC) based on SNMG-40 film shows an ultrahigh energy density of 22.3 Wh kg−1, which is much higher than those previously reported MXene-based materials. Moreover, the aMGSC also provides excellent mechanical durability under different deformation conditions. Thus, this strategy makes MXene materials more competitive for real-world applications such as flexible electronics and electromagnetic interference shielding.  相似文献   

12.
The demand for a new generation of flexible, portable, and high‐capacity power sources increases rapidly with the development of advanced wearable electronic devices. Here we report a simple process for large‐scale fabrication of self‐standing composite film electrodes composed of NiCo2O4@carbon nanotube (CNT) for supercapacitors. Among all composite electrodes prepared, the one fired in air displays the best electrochemical behavior, achieving a specific capacitance of 1,590 F g?1 at 0.5 A g?1 while maintaining excellent stability. The NiCo2O4@CNT/CNT film electrodes are fabricated via stacking NiCo2O4@CNT and CNT alternately through vacuum filtration. Lightweight, flexible, and self‐standing film electrodes (≈24.3 µm thick) exhibit high volumetric capacitance of 873 F cm?3 (with an areal mass of 2.5 mg cm?2) at 0.5 A g?1. An all‐solid‐state asymmetric supercapacitor consists of a composite film electrode and a treated carbon cloth electrode has not only high energy density (≈27.6 Wh kg?1) at 0.55 kW kg?1 (including the weight of the two electrodes) but also excellent cycling stability (retaining ≈95% of the initial capacitance after 5000 cycles), demonstrating the potential for practical application in wearable devices.  相似文献   

13.
2D MXene materials have attracted intensive attention in energy storage application. However, MXene usually undergoes serious face-to-face restacking and inferior stability, significantly preventing its further commercial application. Herein, to suppress the oxidation and self-restacking of MXene, an efficient and fast self-assembly route to prepare a 3D porous oxidation-resistant MXene/graphene (PMG) composite with the assistance of an in situ sacrificial metallic zinc template is demonstrated. The self-assembled 3D porous architecture can effectively prevent the oxidation of MXene layers with no evident variation in electrical conductivity in air at room temperature after two months, guaranteeing outstanding electrical conductivity and abundant electrochemical active sites accessible to electrolyte ions. Consequently, the PMG-5 electrode possesses a striking specific capacitance of 393 F g−1, superb rate performance (32.7% at 10 V s−1), and outstanding cycling stability. Furthermore, the as-assembled asymmetric supercapacitor possesses a pronounced energy density of 50.8 Wh kg−1 and remarkable cycling stability with a 4.3% deterioration of specific capacitance after 10 000 cycles. This work paves a new avenue to solve the two long-standing significant challenges of MXene in the future.  相似文献   

14.
Bismuth (Bi) has attracted considerable attention as promising anode material for sodium-ion batteries (NIBs) owing to its suitable reaction potential and high volumetric capacity density (3750 mA h cm−3). However, the large volumetric expansion during cycling causes severe structural degradation and fast capacity decay. Herein, by rational design, a self-healing nanostructure 3D continuous bulk porous bismuth (3DPBi) is prepared via facile liquid phase reduction reaction. The 3D interconnected Bi nanoligaments provide unblocked electronic circuits and short ion diffusion path. Meanwhile, the bicontinuous nanoporous network can realize self-healing the huge volume variation as confirmed by in situ and ex situ transmission electron microscopy observations. When used as the anode for NIBs, the 3DPBi delivers unprecedented rate capability (high capacity retention of 95.6% at an ultrahigh current density of 60 A g−1 with respect to 1 A g−1) and long-cycle life (high capacity of 378 mA h g−1 remained after 3000 cycles at 10 A g−1). In addition, the full cell of Na3V2(PO4)3|3DPBi delivers stable cycling performance and high gravimetric energy density (116 Wh kg−1), demonstrating its potential in practical application.  相似文献   

15.
Engineering core-shell materials with rationally designed architectures and components is an effective strategy to fulfill the high-performance requirements of supercapacitors. Herein, hierarchical candied-haws-like NiCo2S4@NiCo(HCO3)2 core-shell heterostructure (NiCo2S4@HCs) is designed with NiCo(HCO3)2 polyhedrons being tightly strung by cross-linked NiCo2S4 nanowires. This rational design not only creates more electroactive sites but also suppresses the volume expansion during the charge–discharge processes. Meanwhile, density functional theory calculations ascertain that the formation of NiCo2S4@HCs heterostructure simultaneously facilitates OH adsorption/desorption and accelerates electron transfer within the electrode, boosting fast and efficient redox reactions. Ex situ X-ray diffraction and Raman measurements reveal that gradual phase transformations from NiCo(HCO3)2 to NiCo(OH)2CO3 and then to highly-active NiCoOOH take place during the cycles. Therefore, NiCo2S4@HCs demonstrates an ultrahigh capacitance of 3178.2 F g−1 at 1 A g−1 and a remarkable rate capability of 2179.3 F g−1 at 30 A g−1. In addition, the asymmetric supercapacitor NiCo2S4@HCs//AC exhibits a high energy density of 69.6 W h kg−1 at the power density of 847 W kg−1 and excellent cycling stability with 90.2% retained capacitance after 10 000 cycles. Therefore, this novel structural design has effectively manipulated the interface charge states and guaranteed the structural integrity of electrode materials to achieve superior electrochemical performances.  相似文献   

16.
MXenes, a young family of 2D transition metal carbides/nitrides, show great potential in electrochemical energy storage applications. Herein, a high performance ultrathin flexible solid‐state supercapacitor is demonstrated based on a Mo1.33C MXene with vacancy ordering in an aligned layer structure MXene/poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonic acid) (PEDOT:PSS) composite film posttreated with concentrated H2SO4. The flexible solid‐state supercapacitor delivers a maximum capacitance of 568 F cm?3, an ultrahigh energy density of 33.2 mWh cm?3 and a power density of 19 470 mW cm?3. The Mo1.33C MXene/PEDOT:PSS composite film shows a reduction in resistance upon H2SO4 treatment, a higher capacitance (1310 F cm?3) and improved rate capabilities than both pristine Mo1.33C MXene and the nontreated Mo1.33C/PEDOT:PSS composite films. The enhanced capacitance and stability are attributed to the synergistic effect of increased interlayer spacing between Mo1.33C MXene layers due to insertion of conductive PEDOT, and surface redox processes of the PEDOT and the MXene.  相似文献   

17.
The inferior electrical conductivity of conventional electrodes and their slow charge transport impose limitations on the electrochemical performance of supercapacitors (SCs) using those electrodes, necessitating strategies to overcome the limitations. An in situ Ag ion-incorporated cation-exchanged bimetallic sulfide/metal oxide heterostructure (Ag-Co9-xFexS8@α-FexOy) is synthesized using a two-step hydrothermal method. The coordination bond formation and Ag nanoparticle (NP) incorporation improve the electrical conductivity and adhesion of the heterostructure and reduce its interface resistance and volume expansion throughout the charge/discharge cycles. Density functional theory investigations indicate that the remarkable interlayer and interparticle conductivities of the heterostructure resulting from Ag doping have changed its electronic states, leading to an enhanced electrical conductivity. The optimized electrode has an excellent specific capacity (213.6 mA h g−1 at 1 A g−1) and can maintain 93.2% capacity retention with excellent Coulombic efficiency over 20 000 charge/discharge cycles. A flexible solid-state extrinsic pseudocapacitor (EPSC) is fabricated using Ag-Co9-xFexS8@α-FexOy and Ti3C2TX electrodes. The EPSC has specific and volumetric capacitances of 259 F g−1 and 2.7 F cm−3 at 0.7 A g−1, respectively, an energy density of 80.9 Wh kg−1 at 525 W kg−1, and a capacity retention of 92.8% over 5000 charge/discharge cycles.  相似文献   

18.
Hybrid supercapacitors use electric double-layer capacitance and Faradaic pseudocapacitance as energy storage mechanisms. This type of supercapacitor is becoming a prime candidate for next-generation energy storage devices, with advantages in terms of energy density, specific capacitance, and life cycle. However, reducing the electrode area and increasing the specific capacitance of hybrid supercapacitors remain challenging. In this study, a MoCl5 Precursor-assisted Ultrafast Laser Carbonization (MPAULC) method to fabricate symmetric hybrid supercapacitors with improved capacitance and reduced size is proposed. The method uses an ultrafast laser to induce the formation of carbon/MoO3 composite with the assistance of the MoCl5 precursor. This ultrafast laser carbonization method exhibited high processing precision. The role of the precursor in laser processing is studied using time-resolved imaging and temperature calculations. The specific area capacitance of the C/MoO3 hybrid supercapacitor is 11.85 mF cm−2, 9.2 times higher than that of the laser-induced carbon supercapacitor without precursor. The MPAULC method provides a reliable pathway for fabricating miniaturized hybrid supercapacitors with carbon/metal oxide composite electrodes on polymer substrates.  相似文献   

19.
Fibrous supercapacitor (FSC) is of great attention in wearable electronics, but is challenged by low energy density, owing to disordered diffusion pathway and sluggish redox kinetics. Herein, using micro-reaction strategy, an anisotropic superstructure is developed by in situ anchoring ultrafine zinc sulfine (ZnS) nanoclusters on conductively ordered macro-microporous carbon skeleton via interfacial C S Zn bonds (ZnS/SOM-C). The anisotropic superstructure affords 3D ordered macro-microporous pathways, large accessible surfaces, and highly dispersed active sites, which exhibit enhanced electrolyte mass diffusion, rapid interfacial charge transfer, and large faradaic ions storage (capacitance of 1158 F g−1 in KOH aqueous solution). By microfluidic spinning, the ZnS/SOM-C is further assembled into fibrous electrode of FSC that delivers high capacitance (791 F g−1), commercial-level energy density (172 mWh g−1), and durable stability. As a result, the FSC can realize wearable self-powered applications (e.g., self-cleaning ventilatory mask, smartwatch, and display), exhibiting the superiority in new energy and wearable industry.  相似文献   

20.
Wearable energy storage devices that can be used in the garment industry are strongly required to power E-textiles. In this article, polypyrrole (PPy) nanorods were deposited on cotton fabrics via in situ polymerization of pyrrole in the presence of the fibrillar complex of FeCl3 and methyl orange as a reactive self-degraded template. The obtained fabrics could be directly used as supercapacitor electrodes, with a maximum specific capacitance of 325 F g−1 and an energy density of 24.7 Wh kg−1 at a current density of 0.6 mA cm−2. The capacitance remained higher than 200 F g−1 after 500 cycles.  相似文献   

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