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1.
Aqueous Ni/Fe batteries have great potential as flexible energy storage devices, owing to their low cost, low toxicity, high safety, and high energy density. However, the poor cycling stability has limited the widely expected application of Ni/Fe batteries, while the use of heavy metal substrates cannot meet the basic requirement for flexible devices. In this work, a flexible type of solid‐state Ni/Fe batteries with high energy and power densities is rationally developed using needle‐like Fe3O4 and flake‐like NiO directly grown on carbon cloth/carbon nanofiber (CC–CF) matrix as the anode and cathode, respectively. The hierarchical CC–CF substrate with high electric conductivity and good flexibility serves as an ideal support for guest active materials of nanocrystalline Fe3O4 and NiO, which can effectively buffer the volume change giving rise to good cycling ability. By utilizing a gel electrolyte, a robust and mechanically flexible quasi‐solid‐state Ni/Fe full cell can be assembled. It demonstrates optimal electrochemical performance, such as high energy density (5.2 mWh cm?3 and 94.5 Wh Kg?1), high power density (0.64 W cm?3 and 11.8 KW Kg?1), together with excellent cycling ability. This work provides an example of solid‐state alkaline battery with high electrochemical performance and mechanical flexibility, holding great potential for future flexible electronic devices.  相似文献   

2.
Sodium‐ion batteries are promising for grid‐scale storage applications due to the natural abundance and low cost of sodium. However, few electrodes that can meet the requirements for practical applications are available today due to the limited routes to exploring new materials. Here, a new strategy is proposed through partially/fully substituting the redox couple of existing negative electrodes in their reduced forms to design the corresponding new positive electrode materials. The power of this strategy is demonstrated through the successful design of new tunnel‐type positive electrode materials of Na0.61[Mn0.61‐xFexTi0.39]O2, composed of non‐toxic and abundant elements: Na, Mn, Fe, Ti. In particular, the designed air‐stable Na0.61[Mn0.27Fe0.34Ti0.39]O2 shows a usable capacity of ≈90 mAh g?1, registering the highest value among the tunnel‐type oxides, and a high storage voltage of 3.56 V, corresponding to the Fe3+/Fe4+ redox couple realized for the first time in non‐layered oxides, which was confirmed by X‐ray absorption spectroscopy and Mössbauer spectroscopy. This new strategy would open an exciting route to explore electrode materials for rechargeable batteries.  相似文献   

3.
A challenge still remains to develop high‐performance and cost‐effective air electrode for Li‐O2 batteries with high capacity, enhanced rate capability and long cycle life (100 times or above) despite recent advances in this field. In this work, a new design of binder‐free air electrode composed of three‐dimensional (3D) graphene (G) and flower‐like δ‐MnO2 (3D‐G‐MnO2) has been proposed. In this design, graphene and δ‐MnO2 grow directly on the skeleton of Ni foam that inherits the interconnected 3D scaffold of Ni foam. Li‐O2 batteries with 3D‐G‐MnO2 electrode can yield a high discharge capacity of 3660 mAh g?1 at 0.083 mA cm?2. The battery can sustain 132 cycles at a capacity of 492 mAh g?1 (1000 mAh gcarbon ?1) with low overpotentials under a high current density of 0.333 mA cm?2. A high average energy density of 1350 Wh Kg?1 is maintained over 110 cycles at this high current density. The excellent catalytic activity of 3D‐G‐MnO2 makes it an attractive air electrode for high‐performance Li‐O2 batteries.  相似文献   

4.
Herein, P′2‐type Na0.67[Ni0.1Fe0.1Mn0.8]O2 is introduced as a promising new cathode material for sodium‐ion batteries (SIBs) that exhibits remarkable structural stability during repetitive Na+ de/intercalation. The O? Ni? O? Mn? O? Fe? O bond in the octahedra of transition‐metal layers is used to suppress the elongation of the Mn? O bond and to improve the electrochemical activity, leading to the highly reversible Na storage mechanism. A high discharge capacity of ≈220 mAh g?1 (≈605 Wh kg?1) is delivered at 0.05 C (13 mAg?1) with a high reversible capacity of ≈140 mAh g?1 at 3 C and excellent capacity retention of 80% over 200 cycles. This performance is associated with the reversible P′2–OP4 phase transition and small volume change upon charge and discharge (≈3%). The nature of the sodium storage mechanism in a full cell paired with a hard carbon anode reveals an unexpectedly high energy density of ≈542 Wh kg?1 at 0.2 C and good capacity retention of ≈81% for 500 cycles at 1 C (260 mAg?1).  相似文献   

5.
Na‐based batteries have long been regarded as an inexpensive, sustainable candidate for large‐scale stationary energy storage applications. Unfortunately, the market penetration of conventional Na‐NiCl2 batteries is approaching its limit for several reasons, including limited rate capability and high Ni cost. Herein, a Na‐FeCl2 battery operating at 190 °C is reported that allows a capacity output of 116 mAh g?1 at an extremely high current density of 33.3 mA cm?2 (≈0.6C). The superior rate performance is rooted in the intrinsically fast kinetics of the Fe/Fe2+ redox reaction. Furthermore, it is demonstrated that a small amount of Ni additive (10 mol%) effectively mitigates capacity fading of the Fe/NaCl cathode caused by Fe particle pulverization during long‐term cycling. The modified Fe/Ni cathode exhibits excellent cycling stability, maintaining a discharge energy density of over 295 Wh kg?1 for 200 cycles at 10 mA cm?2 (≈C/5).  相似文献   

6.
Fiber‐shaped aqueous rechargeable Zn batteries (FARZBs) show flexibility, good reliability, cost‐effectiveness, high energy/power densities, and high safety that have attracted increasing attention as promising energy storage devices for future wearable applications. However, the development of FARZB is limited by its poor cycling life and inferior charge–discharge performance, mainly suffering from zinc dendrite growth and increasing electrode irreversibility. In this work, dendrite‐free fiber‐shaped Zn//Co3O4 rechargeable batteries with a long cycle life tested in water and air, are obtained via tuning the surface binding energy of Zn on the anode using the zincophilic N,O‐functional carbon fiber, as well as engineering the Co3O4 cathode with a nanowire array structure. The fiber‐shaped Zn//Co3O4 full battery demonstrates remarkable long cycle life in water and air with high energy density, impressive flexibility, and excellent waterproof ability (fully immersed and charged/discharged under water for more than 33 h for 3000 cycles with capacity retention of ≈80%). The reversible electrochemical mechanisms of the FARZBs, without obvious zinc dendrite deposits and structural change of Co3O4 nanowires, are confirmed by a series of characterizations. These results demonstrate that the FARZBs are promising power sources for emerging wearable electronics.  相似文献   

7.
All‐solid‐state batteries (ASSBs) with silicon anodes are promising candidates to overcome energy limitations of conventional lithium‐ion batteries. However, silicon undergoes severe volume changes during cycling leading to rapid degradation. In this study, a columnar silicon anode (col‐Si) fabricated by a scalable physical vapor deposition process (PVD) is integrated in all‐solid‐state batteries based on argyrodite‐type electrolyte (Li6PS5Cl, 3 mS cm?1) and Ni‐rich layered oxide cathodes (LiNi0.9Co0.05Mn0.05O2, NCM) with a high specific capacity (210 mAh g?1). The column structure exhibits a 1D breathing mechanism similar to lithium, which preserves the interface toward the electrolyte. Stable cycling is demonstrated for more than 100 cycles with a high coulombic efficiency (CE) of 99.7–99.9% in full cells with industrially relevant areal loadings of 3.5 mAh cm?2, which is the highest value reported so far for ASSB full cells with silicon anodes. Impedance spectroscopy revealed that anode resistance is drastically reduced after first lithiation, which allows high charging currents of 0.9 mA cm?2 at room temperature without the occurrence of dendrites and short circuits. Finally, in‐operando monitoring of pouch cells gave valuable insights into the breathing behavior of the solid‐state cell.  相似文献   

8.
Smart construction of ultraflexible electrodes with superior gravimetric and volumetric capacities is still challenging yet significant for sodium ion batteries (SIBs) toward wearable electronic devices. Herein, a hybrid film made of hierarchical Fe1?xS‐filled porous carbon nanowires/reduced graphene oxide (Fe1?xS@PCNWs/rGO) is synthesized through a facile assembly and sulfuration strategy. The resultant hybrid paper exhibits high flexibility and structural stability. The multidimensional paper architecture possesses several advantages, including rendering an efficient electron/ion transport network, buffering the volume expansion of Fe1?xS nanoparticles, mitigating the dissolution of polysulfides, and enabling superior kinetics toward efficient sodium storage. When evaluated as a self‐supporting anode for SIBs, the Fe1?xS@PCNWs/rGO paper electrode exhibits remarkable reversible capacities of 573–89 mAh g?1 over 100 consecutive cycles at 0.1 A g?1 with areal mass loadings of 0.9–11.2 mg cm?2 and high volumetric capacities of 424–180 mAh cm?3 in the current density range of 0.2–5 A g?1. More competitively, a SIB based on this flexible Fe1?xS@PCNWs/rGO anode demonstrates outstanding electrochemical properties, thus highlighting its enormous potential in versatile flexible and wearable applications.  相似文献   

9.
Developing low‐cost, high‐capacity, high‐rate, and robust earth‐abundant electrode materials for energy storage is critical for the practical and scalable application of advanced battery technologies. Herein, the first example of synthesizing 1D peapod‐like bimetallic Fe2VO4 nanorods confined in N‐doped carbon porous nanowires with internal void space (Fe2VO4?NC nanopeapods) as a high‐capacity and stable anode material for potassium‐ion batteries (KIBs) is reported. The peapod‐like Fe2VO4?NC nanopeapod heterostructures with interior void space and external carbon shell efficiently prevent the aggregation of the active materials, facilitate fast transportation of electrons and ions, and accommodate volume variation during the cycling process, which substantially boosts the rate and cycling performance of Fe2VO4. The Fe2VO4?NC electrode exhibits high reversible specific depotassiation capacity of 380 mAh g?1 at 100 mA g?1 after 60 cycles and remarkable rate capability as well as long cycling stability with a high capacity of 196 mAh g?1 at 4 A g?1 after 2300 cycles. The first‐principles calculations reveal that Fe2VO4?NC nanopeapods have high ionic/electronic conductivity characteristics and low diffusion barriers for K+‐intercalation. This study opens up new way for investigating high‐capacity metal oxide as high‐rate and robust electrode materials for KIBs.  相似文献   

10.
A rechargeable, stretchable battery composed of a liquid metal alloy (eutectic gallium‐indium; EGaIn) anode, a carbon paste, and MnO2 slurry cathode, an alkaline electrolytic hydrogel, and a soft elastomeric package is presented. The battery can stably cycle within a voltage range of 1.40–1.86 V at 1 mA cm?2 while being subject to 100% tensile strain. This is accomplished through a mechanism that involves reversible stripping and plating of gallium along with MnO2 chemical conversion. Moreover, a technique to increase the contact area between the EGaIn anode and hydrogel interface using CaCl2 additives, which reduces polarization and therefore reduces the effective current density, leading to higher discharge plateaus and lower charge plateaus. Relative to previous attempts at energy storage with liquid metal, the EGaIn‐MnO2 battery presented here shows an exceptional areal specific capacity (≈3.8 mAh cm?2) and robust, stable rechargeability over >100 charging cycles. The battery is also stable under bending, with negligible change in electrochemical properties when bent to a 2 mm radius of curvature. Batteries embedded within a wearable elastomeric sleeve can power a blue light‐emitting diode and strain‐sensing circuit. These demonstrations suggest that stretchable EGaIn‐MnO2 batteries are feasible for applications in wearable energy‐storage electronics.  相似文献   

11.
Although metallic lithium is regarded as the “Holy Grail” for next‐generation rechargeable batteries due to its high theoretical capacity and low overpotential, the uncontrollable Li dendrite growth, especially under high current densities and deep plating/striping, has inhibited its practical application. Herein, a 3D‐printed, vertically aligned Li anode (3DP‐VALi) is shown to efficiently guide Li deposition via a “nucleation within microchannel walls” process, enabling a high‐performance, dendrite‐free Li anode. Moreover, the microchannels within the microwalls are beneficial for promoting fast Li+ diffusion, supplying large space for the accommodation of Li during the plating/stripping process. The high‐surface‐area 3D anode design enables high operating current densities and high areal capacities. As a result, the Li–Li symmetric cells using 3DP‐VALi demonstrate excellent electrochemical performances as high as 10 mA cm?2/10 mAh cm?2 for 1500 h and 5 mA cm?2/20 mAh cm?2 for 400 h, respectively. Additionally, the Li–S and Li–LiFePO4 cells using 3DP‐VALi anodes present excellent cycling stability up to 250 and 800 cycles at a rate of 1 C, respectively. It is believed that these new findings could open a new window for dendrite‐free metal anode design and pave the way toward energy storage devices with high energy/power density.  相似文献   

12.
Sulfur represents one of the most promising cathode materials for next‐generation batteries; however, the widely observed polysulfide dissolution/shuttling phenomenon in metal–sulfur redox chemistries has severely restricted their applications. Here it is demonstrated that when pairing the sulfur electrode with the iron metal anode, the inherent insolubility of iron sulfides renders the shuttling‐free nature of the Fe–S electrochemical reactions. Consequently, the sulfur electrode exhibits promising performance for Fe2+ storage, where a high capacity of ≈1050 mAh g?1, low polarization of ≈0.16 V as well as stable cycling of 150 cycles are realized. The Fe–S redox mechanism is further revealed as an intriguing stepwise conversion of S8 ? FeS2 ? Fe3S4 ? FeS, where a low volume expansion of ≈32.6% and all‐solid‐state phase transitions facilitate the reaction reversibility. This study suggests an alternative direction to exploit sulfur electrodes in rechargeable transition metal–sulfur batteries.  相似文献   

13.
The application of lithium (Li) metal anodes in Li metal batteries has been hindered by growth of Li dendrites, which lead to short cycling life. Here a Li‐ion‐affinity leaky film as a protection layer is reported to promote a dendrite‐free Li metal anode. The leaky film induces electrokinetic phenomena to enhance Li‐ion transport, leading to a reduced Li‐ion concentration polarization and homogeneous Li‐ion distribution. As a result, the dendrite‐free Li metal anode during Li plating/stripping is demonstrated even at an extremely high deposition capacity (6 mAh cm?2) and current density (40 mA cm?2) with improved Coulombic efficiencies. A full cell battery with the leaky‐film protected Li metal as the anode and high‐areal‐capacity LiNi0.8Co0.1Mn0.1O2 (NCM‐811) (≈4.2 mAh cm?2) or LiFePO4 (≈3.8 mAh cm?2) as the cathode shows improved cycling stability and capacity retention, even at lean electrolyte conditions.  相似文献   

14.
Lithium metal is the most promising anode material for next‐generation batteries, owing to its high theoretical specific capacity and low electrochemical potential. However, the practical application of lithium metal batteries (LMBs) has been plagued by the issues of uncontrollable lithium deposition. The multifunctional nanostructured anode can modulate the initial nucleation process of lithium before the extension of dendrites. By combing the theoretical design and experimental validation, a novel nucleation strategy is developed by introducing sulfur (S) to graphene. Through first‐principles simulations, it is found that S atom doping can improve the Li adsorption ability on a large area around the S doping positions. Consequently, S‐doped graphene with five lithiophilic sites rather than a single atomic site can serve as the pristine nucleation area, reducing the uneven Li deposition and improving the electrochemical performance. Modifying Li metal anodes by S‐doped graphene enables an ultralow overpotential of 5.5 mV, a high average Coulombic efficiency of 99% over more than 180 cycles at a current density of 0.5 mA cm?2 for 1.0 mAh cm?2, and a high areal capacity of 3 mAh cm?2. This work sheds new light on the rational design of nucleation area materials for dendrite‐free LMB.  相似文献   

15.
Inhibiting the shuttle effect of lithium polysulfides and accelerating their conversion kinetics are crucial for the development of high‐performance lithium–sulfur (Li–S) batteries. Herein, a modified template method is proposed to synthesize the robust yolk–shell sulfur host that is constructed by enveloping dispersive Fe2O3 nanoparticles within Mn3O4 nanosheet‐grafted hollow N‐doped porous carbon capsules (Fe2O3@N‐PC/Mn3O4‐S). When applied as a cathode for Li–S batteries, the as‐prepared Fe2O3@N‐PC/Mn3O4‐S can deliver capacities as high as 1122 mAh g?1 after 200 cycles at 0.5 C and 639 mAh g?1 after 1500 cycles at 10 C, respectively. Remarkably, even as the areal sulfur loading is increased to 5.1 mg cm?2, the cathode can still maintain a high areal specific capacity of 5.08 mAh cm?2 with a fading rate of only 0.076% per cycle over 100 cycles at 0.1 C. By a further combination analysis of electron holography and electron energy loss spectroscopy, the outstanding performance is revealed to be mainly traced to the oxygen‐vacancy‐induced interfacial charge field, which immobilizes and catalyzes the conversion of lithium polysulfides, assuring low polarization, fleet redox reaction kinetics, and sufficient utilization of sulfur. These new findings may shed light on the dependence of electrochemical performance on the heterostructure of sulfur hosts.  相似文献   

16.
As the theoretical limit of intercalation material‐based lithium‐ion batteries is approached, alternative chemistries based on conversion reactions are presently considered. The conversion of sulfur is particularly appealing as it is associated with a theoretical gravimetric energy density up to 2510 Wh kg?1. In this paper, three different carbon‐iron disulfide‐sulfur (C‐FeS2‐S) composites are proposed as alternative positive electrode materials for all‐solid‐state lithium‐sulfur batteries. These are synthesized through a facile, low‐cost, single‐step ball‐milling procedure. It is found that the crystalline structure (evaluated by X‐ray diffraction) and the morphology of the composites (evaluated by scanning electron microscopy) are greatly influenced by the FeS2:S ratio. Li/LiI‐Li3PS4/C‐FeS2‐S solid‐state cells are tested under galvanostatic conditions, while differential capacity plots are used to discuss the peculiar electrochemical features of these novel materials. These cells deliver capacities as high as 1200 mAh g(FeS2+S)?1 at the intermediate loading of 1 mg cm?2 (1.2 mAh cm?2), and up to 3.55 mAh cm?2 for active material loadings as high as 5 mg cm?2 at 20 °C. Such an excellent performance, rarely reported for (sulfur/metal sulfide)‐based, all solid‐state cells, makes these composites highly promising for real application where high positive electrode loadings are required.  相似文献   

17.
The symmetric batteries with an electrode material possessing dual cathodic and anodic properties are regarded as an ideal battery configuration because of their distinctive advantages over the asymmetric batteries in terms of fabrication process, cost, and safety concerns. However, the development of high‐performance symmetric batteries is highly challenging due to the limited availability of suitable symmetric electrode materials with such properties of highly reversible capacity. Herein, a triple‐hollow‐shell structured V2O5 (THS‐V2O5) symmetric electrode material with a reversible capacity of >400 mAh g?1 between 1.5 and 4.0 V and >600 mAh g?1 between 0.1 and 3.0 V, respectively, when used as the cathode and anode, is reported. The THS‐V2O5 electrodes assembled symmetric full lithium‐ion battery (LIB) exhibits a reversible capacity of ≈290 mAh g?1 between 2 and 4.0 V, the best performed symmetric energy storage systems reported to date. The unique triple‐shell structured electrode makes the symmetric LIB possessing very high initial coulombic efficiency (94.2%), outstanding cycling stability (with 94% capacity retained after 1000 cycles), and excellent rate performance (over 140 mAh g?1 at 1000 mA g?1). The demonstrated approach in this work leaps forward the symmetric LIB performance and paves a way to develop high‐performance symmetric battery electrode materials.  相似文献   

18.
With the rising demand for flexible and wearable electronic devices, flexible power sources with high energy densities are required to provide a sustainable energy supply. Theoretically, rechargeable, flexible Li‐O2/air batteries can provide extremely high specific energy densities; however, the high costs, complex synthetic methods, and inferior mechanical properties of the available flexible cathodes severely limit their practical applications. Herein, inspired by the structure of human blood capillary tissue, this study demonstrates for the first time the in situ growth of interpenetrative hierarchical N‐doped carbon nanotubes on the surface of stainless‐steel mesh (N‐CNTs@SS) for the fabrication of a self‐supporting, flexible electrode with excellent physicochemical properties via a facile and scalable one‐step strategy. Benefitting from the synergistic effects of the high electronic conductivity and stable 3D interconnected conductive network structure, the Li‐O2 batteries obtained with the N‐CNTs@SS cathode exhibit superior electrochemical performance, including a high specific capacity (9299 mA h g?1 at 500 mA g?1), an excellent rate capability, and an exceptional cycle stability (up to 232 cycles). Furthermore, as‐fabricated flexible Li‐air batteries containing the as‐prepared flexible super‐hydrophobic cathode show excellent mechanical properties, stable electrochemical performance, and superior H2O resistibility, which enhance their potential to power flexible and wearable electronic devices.  相似文献   

19.
A simple and template‐free method for preparing three‐dimensional (3D) porous γ‐Fe2O3@C nanocomposite is reported using an aerosol spray pyrolysis technology. The nanocomposite contains inner‐connected nanochannels and γ‐Fe2O3 nanoparticles (5 nm) uniformly embedded in a porous carbon matrix. The size of γ‐Fe2O3 nanograins and carbon content can be controlled by the concentration of the precursor solution. The unique structure of the 3D porous γ‐Fe2O3@C nanocomposite offers a synergistic effect to alleviate stress, accommodate large volume change, prevent nanoparticles aggregation, and facilitate the transfer of electrons and electrolyte during prolonged cycling. Consequently, the nanocomposite shows high‐rate capability and long‐term cyclability when applied as an anode material for Na‐ion batteries (SIBs). Due to the simple one‐pot synthesis technique and high electrochemical performance, 3D porous γ‐Fe2O3@C nanocomposites have a great potential as anode materials for rechargeable SIBs.  相似文献   

20.
In this paper, a novel freestanding core‐branch negative and positive electrode material through integrating trim aligned Fe2O3 nanoneedle arrays (Fe2O3 NNAs) is first proposed with typical mesoporous structures and NiCo2O4/Ni(OH)2 hybrid nanosheet arrays (NiCo2O4/Ni(OH)2 HNAs) on SiC nanowire (SiC NW) skeletons with outstanding resistance to oxidation and corrosion, good conductivity, and large‐specific surface area. The original built SiC NWs@Fe2O3 NNAs is validated to be a highly capacitive negative electrode (721 F g?1 at 2 A g?1, i.e., 1 F cm?2 at 2.8 mA cm?2), matching well with the similarly constructed SiC NWs@NiCo2O4/Ni(OH)2 HNAs positive electrode (2580 F g?1 at 4 A g?1, i.e., 3.12 F cm?2 at 4.8 mA cm?2). Contributed by the uniquely engineered electrodes, a high‐performance asymmetric supercapacitor (ASC) is developed, which can exhibit a maximum energy density of 103 W h kg?1 at a power density of 3.5 kW kg?1, even when charging the device within 6.5 s, the energy density can still maintain as high as 45 W h kg?1 at 26.1 kW kg?1, and the ASC manifests long cycling lifespan with 86.6% capacitance retention even after 5000 cycles. This pioneering work not only offers an attractive strategy for rational construction of high‐performance SiC NW‐based nanostructured electrodes materials, but also provides a fresh route for manufacturing next‐generation high‐energy storage and conversion systems.  相似文献   

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