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1.
Sodium‐ion batteries (SIBs) have gained tremendous interest for grid scale energy storage system and power energy batteries. However, the current researches of anode for SIBs still face the critical issues of low areal capacity, limited cycle life, and low initial coulombic efficiency for practical application perspective. To solve this issue, a kind of hierarchical 3D carbon‐networks/Fe7S8/graphene (CFG) is designed and synthesized as freestanding anode, which is constructed with Fe7S8 microparticles well‐welded on 3D‐crosslinked carbon‐networks and embedded in highly conductive graphene film, via a facile and scalable synthetic method. The as‐prepared freestanding electrode CFG represents high areal capacity (2.12 mAh cm?2 at 0.25 mA cm?2) and excellent cycle stability of 5000 cycles (0.0095% capacity decay per cycle). The assembled all‐flexible sodium‐ion battery delivers remarkable performance (high areal capacity of 1.42 mAh cm?2 at 0.3 mA cm?2 and superior energy density of 144 Wh kg?1), which are very close to the requirement of practical application. This work not only enlightens the material design and electrode engineering, but also provides a new kind of freestanding high energy density anode with great potential application prospective for SIBs.  相似文献   

2.
Sulfur cathodes have become appealing for rechargeable batteries because of their high theoretical capacity (1675 mA h g?1). However, the conventional cathode configuration borrowed from lithium‐ion batteries may not allow the pure sulfur cathode to put its unique materials chemistry to good use. The solid(sulfur)–liquid(polysulfides)–solid(sulfides) phase transitions generate polysulfide intermediates that are soluble in the commonly used organic solvents in Li–S cells. The resulting severe polysulfide diffusion and the irreversible active‐material loss have been hampering the development of Li–S batteries for years. The present study presents a robust, ultra‐tough, flexible cathode with the active‐material fillings encapsulated between two buckypapers (B), designated as buckypaper/sulfur/buckypaper (B/S/B) cathodes, that suppresses the irreversible polysulfide diffusion to the anode and offers excellent electrochemical reversibility with a low capacity fade rate of 0.06% per cycle after 400 cycles. Engineering enhancements demonstrate that the B/S/B cathodes represent a facile approach for the development of high‐performance sulfur electrodes with a high areal capacity of 5.1 mA h cm?2, which increases further to approach 7 mA h cm?2 on coupling with carbon‐coated separators.  相似文献   

3.
The growing demand for rechargeable lithium‐ion batteries (LIBs) with higher capacity in customized geometries underscores the need for new battery materials, architectures, and assembly strategies. Here, the design, fabrication, and electrochemical performance of fully 3D printed LIBs composed of thick semisolid electrodes that exhibit high areal capacity are reported. Specifically, semisolid cathode and anode inks, as well as UV curable packaging and separator inks for direct writing of LIBs in arbitrary geometries are created. These fully 3D printed and packaged LIBs, which are encased between two glassy carbon current collectors, deliver an areal capacity of 4.45 mAh cm?2 at a current density of 0.14 mA cm?2, which is equivalent to 17.3 Ah L?1. The ability to produce high‐performance LIBs in customized form factors opens new avenues for integrating batteries directly within 3D printed objects.  相似文献   

4.
A crumply and highly flexible lithium‐ion battery is realized by using microfiber mat electrodes in which the microfibers are wound or webbed with conductive nanowires. This electrode architecture guarantees extraordinary mechanical durability without any increase in resistance after folding 1000 times. Its areal energy density is easily controllable by the number of folded stacks of a piece of the electrode mat. Deformable lithium‐ion batteries of lithium iron phosphate as cathode and lithium titanium oxide as anode at high areal capacity (3.2 mAh cm?2) are successfully operated without structural failure and performance loss, even after repeated crumpling and folding during charging and discharging.  相似文献   

5.
High‐capacity anodes of lithium‐ion batteries generally suffer from poor electrical conductivity, large volume variation, and low tap density caused by prepared nanostructures, which make it an obstacle to achieve both high‐areal capacity and stable cycling performance for practical applications. Herein, micrometer‐sized porous Fe2N/C bulk is prepared to tackle the aforementioned issues, and thus realize both high‐areal capacity and stable cycling performance at high mass loading. The porous structure in Fe2N/C bulk is beneficial to alleviate the volumetric change. In addition, the N‐doped carbon conducting networks with high electrical conductivity provide a fast charge transfer pathway. Meanwhile, the micrometer‐sized Fe2N/C bulk exhibits a higher tap density than that of commercial graphite powder (1.03 g cm?3), which facilitates the preparation of thinner electrode at high mass loadings. As a result, a high‐areal capacity of above 4.2 mA h cm?2 at 0.45 mA cm?2 is obtained at a high mass loading of 7.0 mg cm?2 for LIBs, which still maintains at 2.59 mA h cm?2 after 200 cycles with a capacity retention of 98.8% at 0.89 mA cm?2.  相似文献   

6.
Flexible power sources have shown great promise in next‐generation bendable, implantable, and wearable electronic systems. Here, flexible and binder‐free electrodes of Na3V2(PO4)3/reduced graphene oxide (NVP/rGO) and Sb/rGO nanocomposites for sodium‐ion batteries are reported. The Sb/rGO and NVP/rGO paper electrodes with high flexibility and tailorability can be easily fabricated. Sb and NVP nanoparticles are embedded homogenously in the interconnected framework of rGO nanosheets, which provides structurally stable hosts for Na‐ion intercalation and deintercalation. The NVP/rGO paper‐like cathode delivers a reversible capacity of 113 mAh g?1 at 100 mA g?1 and high capacity retention of ≈96.6% after 120 cycles. The Sb/rGO paper‐like anode gives a highly reversible capacity of 612 mAh g?1 at 100 mA g?1, an excellent rate capacity up to 30 C, and a good cycle performance. Moreover, the sodium‐ion full cell of NVP/rGO//Sb/rGO has been fabricated, delivering a highly reversible capacity of ≈400 mAh g?1 at a current density of 100 mA g?1 after 100 charge/discharge cycles. This work may provide promising electrode candidates for developing next‐generation energy‐storage devices with high capacity and long cycle life.  相似文献   

7.
Fast lithium ion transport with a high current density is critical for thick sulfur cathodes, stemming mainly from the difficulties in creating effective lithium ion pathways in high sulfur content electrodes. To develop a high‐rate cathode for lithium–sulfur (Li–S) batteries, extenuation of the lithium ion diffusion barrier in thick electrodes is potentially straightforward. Here, a phyllosilicate material with a large interlamellar distance is demonstrated in high‐rate cathodes as high sulfur loading. The interlayer space (≈1.396 nm) incorporated into a low lithium ion diffusion barrier (0.155 eV) significantly facilitates lithium ion diffusion within the entire sulfur cathode, and gives rise to remarkable nearly sulfur loading‐independent cell performances. When combined with 80% sulfur contents, the electrodes achieve a high capacity of 865 mAh g?1 at 1 mA cm?2 and a retention of 345 mAh g?1 at a high discharging/charging rate of 15 mA cm?2, with a sulfur loading up to 4 mg. This strategy represents a major advance in high‐rate Li–S batteries via the construction of fast ions transfer paths toward real‐life applications, and contributes to the research community for the fundamental mechanism study of loading‐independent electrode systems.  相似文献   

8.
A high capacity cathode is the key to the realization of high‐energy‐density lithium‐ion batteries. The anionic oxygen redox induced by activation of the Li2MnO3 domain has previously afforded an O3‐type layered Li‐rich material used as the cathode for lithium‐ion batteries with a notably high capacity of 250–300 mAh g?1. However, its practical application in lithium‐ion batteries has been limited due to electrodes made from this material suffering severe voltage fading and capacity decay during cycling. Here, it is shown that an O2‐type Li‐rich material with a single‐layer Li2MnO3 superstructure can deliver an extraordinary reversible capacity of 400 mAh g?1 (energy density: ≈1360 Wh kg?1). The activation of a single‐layer Li2MnO3 enables stable anionic oxygen redox reactions and leads to a highly reversible charge–discharge cycle. Understanding the high performance will further the development of high‐capacity cathode materials that utilize anionic oxygen redox processes.  相似文献   

9.
Ultrathick electrode design is a promising strategy to enhance the specific energy of Li‐ion batteries (LIBs) without changing the underlying materials chemistry. However, the low Li‐ion conductivity caused by ultralong Li‐ion transport pathway in traditional random microstructured electrode heavily deteriorates the rate performance of ultrathick electrodes. Herein, inspired by the vertical microchannels in natural wood as the highway for water transport, the microstructures of wood are successfully duplicated into ultrathick bulk LiCoO2 (LCO) cathode via a sol–gel process to achieve the high areal capacity and excellent rate capability. The X‐ray‐based microtomography demonstrates that the uniform microchannels are built up throughout the whole wood‐templated LCO cathode bringing in 1.5 times lower of tortuosity and ≈2 times higher of Li‐ion conductivity compared to that of random structured LCO cathode. The fabricated wood‐inspired LCO cathode delivers high areal capacity up to 22.7 mAh cm?2 (five times of the existing electrode) and achieves the dynamic stress test at such high areal capacity for the first time. The reported wood‐inspired design will open a new avenue to adopt natural hierarchical structures to improve the performance of LIBs.  相似文献   

10.
The design and construction of flexible electrodes that can function at high rates and high areal capacities are essential regarding the practical application of flexible sodium‐ion batteries (SIBs) and other energy storage devices, which remains significantly challenging by far. Herein, a flexible and 3D porous graphene nanosheet/SnS2 (3D‐GNS/SnS2) film is reported as a high‐performance SIB electrode. In this hybrid film, the GNS/SnS2 microblocks serve as pillars to assemble into a 3D porous and interconnected framework, enabling fast electron/ion transport; while the GNS bridges the GNS/SnS2 microblocks into a flexible framework to provide satisfactorily mechanical strength and long‐range conductivity. Moreover, the SnS2 nanocrystals, which chemically bond with GNS, provide sufficient active sites for Na storage and ensure the cycling stability. Consequently, this flexible 3D‐GNS/SnS2 film exhibits excellent Na‐storage performances, especially in terms of high areal capacity (2.45 mAh cm?2) and high rates with superior stability (385 mAh g?1 at 1.0 A g?1 over 1000 cycles with ≈100% retention). A flexible SIB full cell using this anode exhibits high and stable performance under various bending situations. Thus, this work provide a feasible route to prepare flexible electrodes with high practical viability for not only SIBs but also other energy storage devices.  相似文献   

11.
2D metal‐porphyrin frameworks (MPFs) are attractive for advanced energy storage devices. However, the inferior conductivity and low structural stability of MPFs seriously limit their application as flexible free‐standing electrodes with high performance. Here, for the first time, an interlayer hydrogen‐bonded MXene/MPFs film is proposed to overcome these disadvantages by intercalation of highly conductive MXene nanosheets into MPFs nanosheets via a vacuum‐assisted filtration technology. The alternant insertion of MXene and MPFs affords 3D interconnected “MPFs‐to‐MXene‐to‐MPFs” conductive networks to accelerate the ionic/electronic transport rates. Meanwhile, the interlayer hydrogen bonds (F···H? O and O···H? O) contribute a high chemical stability due to a favorable tolerance to volume change caused by phase separation and structural collapse during the charge/discharge process. The synergistic effect makes MXene/MPFs film deliver a capacitance of 326.1 F g?1 at 0.1 A g?1, 1.64 F cm?2 at 1 mA cm?2, 694.2 F cm?3 at 1 mA cm?3 and a durability of about 30 000 cycles. The flexible symmetric supercapacitor shows an areal capacitance of 408 mF cm?2, areal energy density of 20.4 µW h cm?2, and capacitance retention of 95.9% after 7000 cycles. This work paves an avenue for the further exploration of 2D MOFs in flexible energy storage devices.  相似文献   

12.
Storing more energy in a limited device area is very challenging but crucial for the applications of flexible and wearable electronics. Metal vanadates have been regarded as a fascinating group of materials in many areas, especially in lithium‐ion storage. However, there has not been a versatile strategy to synthesize flexible metal vanadate hybrid nanostructures as binder‐free anodes for Li‐ion batteries so far. A convenient and versatile synthesis of MxVyOx+2.5y@carbon cloth (M = Mn, Co, Ni, Cu) composites is proposed here based on a two‐step hydrothermal route. As‐synthesized products demonstrate hierarchical proliferous structure, ranging from nanoparticles (0D), and nanobelts (1D) to a 3D interconnected network. The metal vanadate/carbon hybrid nanostructures exhibit excellent lithium storage capability, with a high areal specific capacity up to 5.9 mAh cm?2 (which equals to 1676.8 mAh g?1) at a current density of 200 mA g?1. Moreover, the nature of good flexibility, mixed valence states, and ultrahigh mass loading density (over 3.5 mg cm?2) all guarantee their great potential in compact energy storage for future wearable devices and other related applications.  相似文献   

13.
Transition metal hydro/oxides (TMH/Os) are treated as the most promising alternative supercapacitor electrodes thanks to their high theoretical capacitance due to the various oxidation states and abundant cheap resources of TMH/Os. However, the poor conductivity and logy reaction kinetics of TMH/Os severely restrict their practical application. Herein, hierarchical core–shell P‐Ni(OH)2@Co(OH)2 micro/nanostructures are in situ grown on conductive Ni foam (P‐Ni(OH)2@Co(OH)2/NF) through a facile stepwise hydrothermal process. The unique heterostructure composed of P‐Ni(OH)2 rods and Co(OH)2 nanoflakes boost the charge transportation and provide abundant active sites when used as the intergrated cathode for supercapacitors. It delivers an ultrahigh areal specific capacitance of 4.4 C cm?2 at 1 mA cm?2 and the capacitance can maintain 91% after 10 000 cycles, showing an ultralong cycle life. Additionally, a hybrid supercapacitor composed with P‐Ni(OH)2@Co(OH)2/NF cathode and Fe2O3/CC anode shows a wider voltage window of 1.6 V, a remarkable energy density of 0.21 mWh cm?2 at the power density of 0.8 mW cm?2, and outstanding cycling stability with about 81% capacitance retention after 5000 cycles. This innovative study not only supplies a newfashioned electronic apparatus with high‐energy density and cycling stability but offers a fresh reference and enlightenment for synthesizing advanced integrated electrodes for high‐performance hybrid supercapacitors.  相似文献   

14.
Suppressing the dendrite formation and managing the volume change of lithium (Li) metal anode have been global challenges in the lithium batteries community. Herein, a duplex copper (Cu) foil with an ant‐nest‐like network and a dense substrate is reported for an ultrastable Li metal anode. The duplex Cu is fabricated by sulfurization of thick Cu foil with a subsequent skeleton self‐welding procedure. Uniform Li deposition is achieved by the 3D interconnected architecture and lithiophilic surface of self‐welded Cu skeleton. The sufficient space in the porous layer enables a large areal capacity for Li and significantly improves the electrode–electrolyte interface. Simulations reveal that the structure allows proper electric field penetration into the connected tunnels. The assembled Li anodes exhibit high coulombic efficiency (97.3% over 300 cycles) and long lifespan (>880 h) at a current density of 1 mA cm?2 with a capacity of 1 mAh cm?2. Stable and deep cycling can be maintained up to 50 times at a high capacity of 10 mAh cm?2.  相似文献   

15.
Facile charge transport by a hydrophilic organic radical‐substituted polymer and the 3D current collection by a self‐assembled mesh of single‐walled carbon nanotube bundles lead to the operation of an ultrahigh‐output rechargeable electrode. Exceptionally large current density beyond 1 A cm?2 and high areal capacity around 3 mAh cm?2 are achieved, which are 101?2 times larger than those of the previously reported so‐called “ultrafast electrodes.” A sub‐millimeter‐thick, flexible, highly safe organic redox polymer‐based rechargeable device with an aqueous sodium chloride electrolyte is fabricated to demonstrate the superior performance.  相似文献   

16.
All‐solid‐state Li–S batteries are promising candidates for next‐generation energy‐storage systems considering their high energy density and high safety. However, their development is hindered by the sluggish electrochemical kinetics and low S utilization due to high interfacial resistance and the electronic insulating nature of S. Herein, Se is introduced into S cathodes by forming SeSx solid solutions to modify the electronic and ionic conductivities and ultimately enhance cathode utilization in all‐solid‐state lithium batteries (ASSLBs). Theoretical calculations confirm the redistribution of electron densities after introducing Se. The interfacial ionic conductivities of all achieved SeSx–Li3PS4 (x = 3, 2, 1, and 0.33) composites are 10?6 S cm?1. Stable and highly reversible SeSx cathodes for sulfide‐based ASSLBs can be developed. Surprisingly, the SeS2/Li10GeP2S12–Li3PS4/Li solid‐state cells exhibit excellent performance and deliver a high capacity over 1100 mAh g?1 (98.5% of its theoretical capacity) at 50 mA g?1 and remained highly stable for 100 cycles. Moreover, high loading cells can achieve high areal capacities up to 12.6 mAh cm?2. This research deepens the understanding of Se–S solid solution chemistry in ASSLB systems and offers a new strategy to achieve high‐performance S‐based cathodes for application in ASSLBs.  相似文献   

17.
The Li–CO2 battery is a promising energy storage device for wearable electronics due to its long discharge plateau, high energy density, and environmental friendliness. However, its utilization is largely hindered by poor cyclability and mechanical rigidity due to the lack of a flexible and durable catalyst electrode. Herein, flexible fiber‐shaped Li–CO2 batteries with ultralong cycle‐life, high rate capability, and large specific capacity are fabricated, employing bamboo‐like N‐doped carbon nanotube fiber (B‐NCNT) as flexible, durable metal‐free catalysts for both CO2 reduction and evolution reactions. Benefiting from high N‐doping with abundant pyridinic groups, rich defects, and active sites of the periodic bamboo‐like nodes, the fabricated Li–CO2 battery shows outstanding electrochemical performance with high full‐discharge capacity of 23 328 mAh g?1, high rate capability with a low potential gap up to 1.96 V at a current density of 1000 mA g?1, stability over 360 cycles, and good flexibility. Meanwhile, the bifunctional B‐NCNT is used as the counter electrode for a fiber‐shaped dye‐sensitized solar cell to fabricate a self‐powered fiber‐shaped Li–CO2 battery with overall photochemical–electric energy conversion efficiency of up to 4.6%. Along with a stable voltage output, this design demonstrates great adaptability and application potentiality in wearable electronics with a breath monitor as an example.  相似文献   

18.
Lithium–sulfur batteries, as one of promising next‐generation energy storage devices, hold great potential to meet the demands of electric vehicles and grids due to their high specific energy. However, the sluggish kinetics and the inevitable “shuttle effect” severely limit the practical application of this technology. Recently, design of composite cathode with effective catalysts has been reported as an essential way to overcome these issues. In this work, oxygen‐deficient ferric oxide (Fe2O3?x), prepared by lithiothermic reduction, is used as a low‐cost and effective cathodic catalyst. By introducing a small amount of Fe2O3?x into the cathode, the battery can deliver a high capacity of 512 mAh g?1 over 500 cycles at 4 C, with a capacity fade rate of 0.049% per cycle. In addition, a self‐supporting porous S@KB/Fe2O3?x cathode with a high sulfur loading of 12.73 mg cm?2 is prepared by freeze‐drying, which can achieve a high areal capacity of 12.24 mAh cm?2 at 0.05 C. Both the calculative and experimental results demonstrate that the Fe2O3?x has a strong adsorption toward soluble polysulfides and can accelerate their subsequent conversion to insoluble products. As a result, this work provides a low‐cost and effective catalyst candidate for the practical application of lithium–sulfur batteries.  相似文献   

19.
In this work, hydroxyl‐functionalized Mo2C‐based MXene nanosheets are synthesized by facilely removing the Sn layer of Mo2SnC. The hydroxyl‐functionalized surface of Mo2C suppresses the shuttle effect of lithium polysulfides (LiPSs) through strong interaction between Mo atoms on the MXenes surface and LiPSs. Carbon nanotubes (CNTs) are further introduced into Mo2C phase to enlarge the specific surface area of the composite, improve its electronic conductivity, and alleviate the volume change during discharging/charging. The strong surface‐bound sulfur in the hierarchical Mo2C‐CNTs host can lead to a superior electrochemical performance in lithium–sulfur batteries. A large reversible capacity of ≈925 mAh g ? 1 is observed after 250 cycles at a current density of 0.1 C (1 C = 1675 mAh g?1) with good rate capability. Notably, the electrodes with high loading amounts of sulfur can also deliver good electrochemical performances, i.e., initial reversible capacities of ≈1314 mAh g?1 (2.4 mAh cm?2), ≈1068 mAh g?1 (3.7 mAh cm?2), and ≈959 mAh g?1 (5.3 mAh cm?2) at various areal loading amounts of sulfur (1.8, 3.5, and 5.6 mg cm?2) are also observed, respectively.  相似文献   

20.
The nonaqueous lithium oxygen battery is a promising candidate as a next‐generation energy storage system because of its potentially high energy density (up to 2–3 kW kg?1), exceeding that of any other existing energy storage system for storing sustainable and clean energy to reduce greenhouse gas emissions and the consumption of nonrenewable fossil fuels. To achieve high energy density, long cycling stability, and low cost, the air electrode structure and the electrocatalysts play important roles. Here, a metal‐free, free‐standing macroporous graphene@graphitic carbon nitride (g‐C3N4) composite air cathode is first reported, in which the g‐C3N4 nanosheets can act as efficient electrocatalysts, and the macroporous graphene nanosheets can provide space for Li2O2 to deposit and also promote the electron transfer. The electrochemical results on the graphene@g‐C3N4 composite air electrode show a 0.48 V lower charging plateau and a 0.13 V higher discharging plateau than those of pure graphene air electrode, with a discharge capacity of nearly 17300 mA h g?1 (composite). Excellent cycling performance, with terminal voltage higher than 2.4 V after 105 cycles at 1000 mA h g?1 (composite) capacity, can also be achieved. Therefore, this hybrid material is a promising candidate for use as a high energy, long‐cycle‐life, and low‐cost cathode material for lithium oxygen batteries.  相似文献   

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