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1.
The energy densities of most supercapacitors (SCs) are low, hindering their practical applications. To construct SCs with ultrahigh energy densities, a porous titanium carbide (TiC)/boron‐doped diamond (BDD) composite electrode is synthesized on a titanium plate that is pretreated using a plasma electrolytic oxidation (PEO) technique. The porous and nanometer‐thick TiO2 layer formed during PEO process prevents the formation of brittle titanium hydride and enhances the BDD growth during chemical vapor deposition processes. Meanwhile, the in situ conversion of TiO2 into TiC is achieved. Combination of this capacitor electrode with soluble redox electrolytes leads to the fabrication of high‐performance SCs in both aqueous and organic solutions. In 0.05 m Fe(CN)63?/4? + 1 m Na2SO4 aqueous solution, the capacitance is as high as 46.3 mF cm?2 at a current density of 1 mA cm?2; this capacitance remains 92% of its initial value even after 10 000 charge/discharge cycles; the energy density is up to 47.4 Wh kg?1 at a power density of 2236 W kg?1. The performance of constructed SCs is superior to most available SCs and some electrochemical energy storage devices like batteries. Such a porous capacitor electrode is thus promising for the construction of high‐performance SCs for practical applications.  相似文献   

2.
Lithium‐oxygen batteries represent a significant scientific challenge for high‐rate and long‐term cycling using oxygen electrodes that contain efficient electrocatalysts. The mixed transition metal oxide catalysts provide the most efficient catalytic activity for partial heterogeneous surface cations with oxygen vacancies as the active phase. They include multiple oxidation states and oxygen vacancies. Here, using a combination of transmission electron microscopy, differential electrochemical mass spectrometry, X‐ray photoelectron spectroscopy, and electrochemical properties to probe the surface of the MnMoO4 nanowires, it is shown that the intrinsic MnMoO4 oxygen vacancies on the oxygen electrode are an effective strategy to achieve a high reversibility and high efficiency for lithium‐oxygen (Li‐O2) batteries. The modified MnMoO4 nanowires exhibit a highly stable capacity at a fixed capacity of 5000 mA h gsp?1 (calculated weight of Super P carbon black) during 50 cycles, a high‐rate capability at a current rate of 3000 mA gsp?1 during 70 cycles, and a long‐term reversible capacity during 188 cycles at a fixed capacity of 1000 mA h gsp?1. It is demonstrated that this strategy for creating mixed transition metal oxides (e.g., MnMoO4) may pave the way for the new structural design of electrocatalysts for Li‐O2 batteries.  相似文献   

3.
Remarkable improvements in the electrochemical performance of Si materials for Li‐ion batteries have been recently achieved, but the inherent volume change of Si still induces electrode expansion and external cell deformation. Here, the void structure in Si‐encapsulating hollow carbons is optimized in order to minimize the volume expansion of Si‐based anodes and improve electrochemical performance. When compared to chemical etching, the hollow structure is achieved via electroless etching is more advanced due to the improved electrical contact between carbon and Si. Despite the very thick electrodes (30 ~ 40 μm), this results in better cycle and rate performances including little capacity fading over 50 cycles and 1100 mA h g?1 at 2C rate. Also, an in situ dilatometer technique is used to perform a comprehensive study of electrode thickness change, and Si‐encapsulating hollow carbon mitigates the volume change of electrodes by adoption of void space, resulting in a small volume increase of 18% after full lithiation corresponding with a reversible capacity of about 2000 mA h g?1.  相似文献   

4.
Rational structure design of the current collector along with further engineering of the solid‐electrolyte interphases (SEI) layer is one of the most promising strategies to achieve uniform Li deposition and inhibit uncontrolled growth of Li dendrites. Here, a Li2S layer as an artificial SEI with high compositional uniformity and high lithium ion conductivity is in situ generated on the surface of the 3D porous Cu current collector to regulate homogeneous Li plating/stripping. Both simulations and experiments demonstrate that the Li2S protective layer can passivate the porous Cu skeleton and balance the transport rate of lithium ions and electrons, thereby alleviating the agglomerated Li deposition at the top of the electrode or at the defect area of the SEI layer. As a result, the modified current collector exhibits long‐term cycling of 500 cycles at 1 mA cm?2 and stable electrodeposition capabilities of 4 mAh cm?2 at an ultrahigh current density of 4 mA cm?2. Furthermore, full batteries (LiFePO4 as cathode) paired with this designed 3D anode with only ≈200% extra lithium show superior stability and rate performance than the batteries paired with lithium foil (≈3000% extra lithium). These explorations provide new strategies for developing high‐performance Li metal anodes.  相似文献   

5.
In this work, a hierarchically porous and ultrathick “breathable” wood‐based cathode for high‐performance Li‐O2 batteries is developed. The 3D carbon matrix obtained from the carbonized and activated wood (denoted as CA‐wood) serves as a superconductive current collector and an ideal porous host for accommodating catalysts. The ruthenium (Ru) nanoparticles are uniformly anchored on the porous wall of the aligned microchannels (denoted as CA‐wood/Ru). The aligned open microchannels inside the carbon matrix contribute to unimpeded oxygen gas diffusion. Moreover, the hierarchical pores on the microchannel walls can be facilely impregnated by electrolyte, forming a continuous supply of electrolyte. As a result, numerous ideal triphase active sites are formed where electrolyte, oxygen, and catalyst accumulate on the porous walls of microchannels. Benefiting from the numerous well‐balanced triple‐phase active sites, the assembled Li‐O2 battery with the CA‐wood/Ru cathode (thickness: ≈700 µm) shows a high specific area capacity of 8.58 mA h cm?2 at 0.1 mA cm?2. Moreover, the areal capacity can be further increased to 56.0 mA h cm?2 by using an ultrathick CA‐wood/Ru cathode with a thickness of ≈3.4 mm. The facile ultrathick wood‐based cathodes can be applied to other cathodes to achieve a super high areal capacity without sacrificing the electrochemical performance.  相似文献   

6.
Fiber‐shaped rechargeable batteries hold promise as the next‐generation energy storage devices for wearable electronics. However, their application is severely hindered by the difficulty in fabrication of robust fiber‐like electrodes with promising electrochemical performance. Herein, yolk–shell NiS2 nanoparticles embedded in porous carbon fibers (NiS2?PCF) are successfully fabricated and developed as high‐performance fiber electrodes for sodium storage. Benefiting from the robust embedded structure, 3D porous and conductive carbon network, and yolk–shell NiS2 nanoparticles, the as‐prepared NiS2?PCF fiber electrode achieves a high reversible capacity of about 679 mA h g?1 at 0.1 C, outstanding rate capability (245 mA h g?1 at 10 C), and ultrastable cycle performance with 76% capacity retention over 5000 cycles at 5 C. Notably, a flexible fiber‐shaped sodium battery is assembled, and high reversible capacity is kept at different bending states. This work offers a new electrode‐design paradigm toward novel carbon fiber electrodes embedded with transition metal oxides/sulfides/phosphides for application in flexible energy storage devices.  相似文献   

7.
NaVPO4F has received a great deal of attention as cathode material for Na‐ion batteries due to its high theoretical capacity (143 mA h g?1), high voltage platform, and structural stability. Novel NaVPO4F/C nanofibers are successfully prepared via a feasible electrospinning method and subsequent heat treatment as self‐standing cathode for Na‐ion batteries. Based on the morphological and microstructural characterization, it can be seen that the NaVPO4F/C nanofibers are smooth and continuous with NaVPO4F nanoparticles (≈6 nm) embedded in porous carbon matrix. For Na‐storage, this electrode exhibits extraordinary electrochemical performance: a high capacity (126.3 mA h g?1 at 1 C), a superior rate capability (61.2 mA h g?1 at 50 C), and ultralong cyclability (96.5% capacity retention after 1000 cycles at 2 C). 1D NaVPO4F/C nanofibers that interlink into 3D conductive network improve the conductivity of NaVPO4F, and effectively restrain the aggregation of NaVPO4F particles during charge/discharge process, leading to the high performance.  相似文献   

8.
High energy‐density, low‐cost batteries are critically important to a variety of applications ranging from portable electronics to electric vehicles (EVs) and grid‐scale storage. While tremendous research effort has been focused on new materials or chemistries with high energy‐density potential, design innovations such as low‐tortuosity thick electrodes are another promising path toward higher energy density and lower cost. Growing demand for fast‐charging batteries has also highlighted the need for negative electrodes that can accept high rate charging without metal deposition; low tortuosity can be a benefit in this regard. However, a general and scalable fabrication method for low‐tortuosity electrodes is currently lacking. Here an emulsion‐based, magnetic‐alignment approach to producing thick electrodes (>400 µm thickness) with ultrahigh areal capacity (up to ≈14 mAh cm?2 vs 2–4 mAh cm?2 for conventional lithium ion) is reported. The process is demonstrated for LiCoO2 and meso‐carbon microbead graphite. The LiCoO2 cathodes are confirmed to have low tortuosity via DC‐depolarization experiments and deliver high areal capacity (>10 mAh cm?2) in galvanostatic discharge tests at practical C‐rates and model EV drive‐cycle tests. This simple fabrication method can potentially be applied to many other active materials to enable thick, low‐tortuosity electrodes.  相似文献   

9.
Achieving a high areal capacity is essential for the transfer of outstanding laboratory electrode results to commercial applications and also to ensure there exists a capacity matched cathode and anode for a properly tuned battery. Despite intensive efforts, most electrode materials exhibit areal capacities lower than that of the graphite anodes (4 mA h cm?2). An effective and low‐cost approach is reported to attain a high areal capacity via an intense densification by compacting a porous carbon nanotube sponge grafted with Co3O4 nanoparticles. The hybrid sponge can be compacted to a large degree (up to a tenfold densification) while still keeping its structural integrity and the 3D porous network. This method allows achieving a mass loading of up ?to 14.3 mg cm?2 and an areal capacity of 12 mA h cm?2 (at a current density of 200 mA g?1) together with a gravimetric capacity of >800 mA h g?1. This densification by compaction approach offers an effective and low‐cost strategy to develop high mass loading and areal capacity electrodes for practical energy storage systems.  相似文献   

10.
Printed batteries are an emerging solution for integrated energy storage using low‐cost, high accuracy fabrication techniques. While several printed batteries have been previously shown, few have designed a battery that can be incorporated into an integrated device. Specifically, a fully printed battery with a small active electrode area (<1 cm2) achieving high areal capacities (>10 mAh cm?2) at high current densities (1–10 mA cm?2) has not been demonstrated, which represents the minimum form‐factor and performance requirements for many low‐power device applications. This work addresses these challenges by investigating the scaling limits of a fully printed Zn–Ag2O battery and determining the electrochemical limitations for a mm2‐scale battery. Processed entirely in air, Zn–Ag2O batteries are well suited for integration in typical semiconductor packaging flows compared to lithium‐based chemistries. Printed cells with electrodes as small as 1 mm2 maintain steady operating voltages above (>1.4 V) at high current densities (1–12 mA cm?2) and achieve the highest reported areal capacity for a fully printed battery at 11 mAh cm?2. The findings represent the first demonstration of a small, packaged, fully printed Zn–Ag2O battery with high areal capacities at high current densities, a crucial step toward realizing chip‐scale energy storage for integrated electronic systems.  相似文献   

11.
Identifying suitable electrode materials for sodium‐ion and potassium‐ion storage holds the key to the development of earth‐abundant energy‐storage technologies. This study reports an anode material based on self‐assembled hierarchical spheroid‐like KTi2(PO4)3@C nanocomposites synthesized via an electrospray method. Such an architecture synergistically combines the advantages of the conductive carbon network and allows sufficient space for the infiltration of the electrolyte from the porous structure, leading to an impressive electrochemical performance, as reflected by the high reversible capacity (283.7 mA h g?1 for Na‐ion batteries; 292.7 mA h g?1 for K‐ion batteries) and superior rate capability (136.1 mA h g?1 at 10 A g?1 for Na‐ion batteries; 133.1 mA h g?1 at 1 A g?1 for K‐ion batteries) of the resulting material. Moreover, the different ion diffusion behaviors in the two systems are revealed to account for the difference in rate performance. These findings suggest that KTi2(PO4)3@C is a promising candidate as an anode material for sodium‐ion and potassium‐ion batteries. In particular, the present synthetic approach could be extended to other functional electrode materials for energy‐storage materials.  相似文献   

12.
For mass production of all‐solid‐state lithium‐ion batteries (ASLBs) employing highly Li+ conductive and mechanically sinterable sulfide solid electrolytes (SEs), the wet‐slurry process is imperative. Unfortunately, the poor chemical stability of sulfide SEs severely restrict available candidates for solvents and in turn polymeric binders. Moreover, the binders interrupt Li+‐ionic contacts at interfaces, resulting in the below par electrochemical performance. In this work, a new scalable slurry fabrication protocol for sheet‐type ASLB electrodes made of Li+‐conductive polymeric binders is reported. The use of intermediate‐polarity solvent (e.g., dibromomethane) for the slurry allows for accommodating Li6PS5Cl and solvate‐ionic‐liquid‐based polymeric binders (NBR‐Li(G3)TFSI, NBR: nitrile?butadiene rubber, G3: triethylene glycol dimethyl ether, LiTFSI: lithium bis(trifluoromethanesulfonyl)imide) together without suffering from undesirable side reactions or phase separation. The LiNi0.6Co0.2Mn0.2O2 and Li4Ti5O12 electrodes employing NBR‐Li(G3)TFSI show high capacities of 174 and 160 mA h g?1 at 30 °C, respectively, which are far superior to those using conventional NBR (144 and 76 mA h g?1). Moreover, high areal capacity of 7.4 mA h cm?2 is highlighted for the LiNi0.7Co0.15Mn0.15O2 electrodes with ultrahigh mass loading of 45 mg cm?2. The facilitated Li+‐ionic contacts at interfaces paved by NBR‐Li(G3)TFSI are evidenced by the complementary analysis from electrochemical and 7Li nuclear magnetic resonance measurements.  相似文献   

13.
Fast developments and substantial achievements have been shaping the field of wearable electronic devices, resulting in the persistent requirement for stretchable lithium‐ion batteries (LIBs). Despite recent progress in stretchable electrodes, stretching full batteries, including electrodes, separator, and sealing material, remains a great challenge. Here, a simple design concept for stretchable LIBs via a wavy structure at the full battery device scale is reported. All components including the package are capable of being reversibly stretched by folding the entire pouch cell into a wavy shape with polydimethylsiloxane filled in each valley region. In addition, the stretchable, sticky, and porous polyurethane/poly(vinylidene fluoride) membrane is adopted as a separator for the first time, which can maintain intimate contact between electrodes and separator to continuously secure ion pathway under dynamic state. Commercial cathode, anode, and package can be utilized in this rationally designed wavy battery to enable stretchability. The results indicate good electrochemical performances and long‐term stability at repeatable release–stretch cycles. A high areal capacity of 3.6 mA h cm?2 and energy density of up to 172 W h L?1 can be achieved for the wavy battery. The promising results of the cost‐effective wavy battery with high stretchability shed light on the development of stretchable energy storages.  相似文献   

14.
This study proposes a conformal surface coating of conducting polymer for protecting 1D nanostructured electrode material, thereby enabling a free‐standing electrode without binder for sodium ion batteries. Here, polypyrrole (PPy), which is one of the representative conducting polymers, encapsulated cobalt phosphide (CoP) nanowires (NWs) grown on carbon paper (CP), finally realizes 1D core–shell CoP@PPy NWs/CP. The CoP core is connected to the PPy shell via strong chemical bonding, which can maintain a Co–PPy framework during charge/discharge. It also possesses bifunctional features that enhances the charge transfer and buffers the volume expansion. Consequently, 1D core–shell CoP@PPy NWs/CP demonstrates superb electrochemical performance, delivering a high areal capacity of 0.521 mA h cm?2 at 0.15 mA cm?2 after 100 cycles, and 0.443 mA h cm?2 at 1.5 mA cm?2 even after 1000 cycles. Even at a high current density of 3 mA cm?2, a significant areal discharge capacity reaching 0.285 mA h cm?2 is still maintained. The outstanding performance of the CoP@PPy NWs/CP free‐standing anode provides not only a novel insight into the modulated volume expansion of anode materials but also one of the most effective strategies for binder‐free and free‐standing electrodes with decent mechanical endurance for future secondary batteries.  相似文献   

15.
The growing demand for advanced energy storage devices with high energy density and high safety has continuously driven the technical upgrades of cell architectures as well as electroactive materials. Designing thick electrodes with more electroactive materials is a promising strategy to improve the energy density of lithium‐ion batteries (LIBs) without alternating the underlying chemistry. However, the progress toward thick, high areal capacity electrodes is severely limited by the sluggish electronic/ionic transport and easy deformability of conventional electrodes. A self‐supported ultrahigh‐capacity and fire‐resistant LiFePO4 (UCFR‐LFP)‐based nanocomposite cathode is demonstrated here. Benefiting from the structural and chemical uniqueness, the UCFR‐LFP electrodes demonstrate exceptional improvements in electrochemical performance and mass loading of active materials, and thermal stability. Notably, an ultrathick UCFR‐LFP electrode (1.35 mm) with remarkably high mass loading of active materials (108 mg cm?2) and areal capacity (16.4 mAh cm?2) is successfully achieved. Moreover, the 1D inorganic binder‐like ultralong hydroxyapatite nanowires (HAP NWs) enable the UCFR‐LFP electrode with excellent thermal stability (structural integrity up to 1000 °C and electrochemical activity up to 750 °C), fire‐resistance, and wide‐temperature operability. Such a unique UCFR‐LFP electrode offers a promising solution for next‐generation LIBs with high energy density, high safety, and wide operating‐temperature window.  相似文献   

16.
A seawater splitting photoelectrochemical cell featuring a nanostructured tungsten trioxide photoanode that exhibits very high and stable photocurrents producing chlorine with average 70% Faradaic efficiency is described. Fabrication of the WO3 electrodes on fluorine‐doped tin oxide substrates involves a simple solution‐based method and sequential layer‐by‐layer deposition with a progressively adjusted amount of structure‐directing agent in the precursor and a two‐step annealing. Such a procedure allows tailoring of thick, highly porous, structurally stable WO3 films with a large internal photoactive surface area optimizing utilization of visible light wavelengths by the photoanode. With the application of an anodic potential of 0.76 V versus Ag/AgCl reference electrode (0.4 V below the thermodynamic Cl2/Cl? potential) in synthetic seawater, the designed WO3 photoanodes irradiated with simulated 1 sun AM 1.5G light reach currents exceeding 4.5 mA cm?2. Photocurrents close to 5 mA cm?2 are attained in the case of fresh water splitting using 1 m methane–sulfonic acid supporting electrolyte with oxygen evolved at the WO3 photoanode. The amount of formed hydrogen is determined by discharging the palladium sheet electrode employed as a cathode. Collection of hydrogen in the form of a hydride opens, more generally, the prospect of subsequently using such materials as anodes in batteries employing oxygen reduction cathodes.  相似文献   

17.
While stretchable micro‐supercapacitors (MSCs) have been realized, they have suffered from limited areal electrochemical performance, thus greatly restricting their practical electronic application. Herein, a facile strategy of 3D printing and unidirectional freezing of a pseudoplastic nanocomposite gel composed of Ti3C2Tx MXene nanosheets, manganese dioxide nanowire, silver nanowires, and fullerene to construct intrinsically stretchable MSCs with thick and honeycomb‐like porous interdigitated electrodes is introduced. The unique architecture utilizes thick electrodes and a 3D porous conductive scaffold in conjunction with interacting material properties to achieve higher loading of active materials, larger interfacial area, and faster ion transport for significantly improved areal energy and power density. Moreover, the oriented cellular scaffold with fullerene‐induced slippage cell wall structure prompts the printed electrode to withstand large deformations without breaking or exhibiting obvious performance degradation. When imbued with a polymer gel electrolyte, the 3D‐printed MSC achieves an unprecedented areal capacitance of 216.2 mF cm?2 at a scan rate of 10 mV s?1, and remains stable when stretched up to 50% and after 1000 stretch/release cycles. This intrinsically stretchable MSC also exhibits high rate capability and outstanding areal energy density of 19.2 µWh cm?2 and power density of 58.3 mW cm?2, outperforming all reported stretchable MSCs.  相似文献   

18.
Lithium‐sulfur (Li‐S) batteries are considered to be one of the promising next‐generation energy storage systems. Considerable progress has been achieved in sulfur composite cathodes, but high cycling stability and discharging capacity at the expense of volumetric capacity have offset their advantages. Herein, a functional separator is presented by coating cobalt‐embedded nitrogen‐doped porous carbon nanosheets and graphene on one surface of a commercial polypropylene separator. The coating layer not only suppresses the polysulfide shuttle effect through chemical affinity, but also functions as an electrocatalyst to propel catalytic conversion of intercepted polysulfides. The slurry‐bladed carbon nanotubes/sulfur cathode with 90 wt% sulfur deliver high reversible capacity of 1103 mA h g?1 and volumetric capacity of 1062 mA h cm?3 at 0.2 C, and the freestanding carbon nanofibers/sulfur cathode provides a high discharging capacity of 1190 mA h g?1 and volumetric capacity of 1136 mA h cm?3 at high sulfur content of 78 wt% and sulfur loading of 10.5 mg cm?2. The electrochemical performance is comparable with or even superior to those in the state‐of‐the‐art carbon‐based sulfur cathodes. The separator reported in this work holds great promise for the development of high‐energy‐density Li‐S batteries.  相似文献   

19.
Uncontrolled dendrites resulting from nonuniform lithium (Li) nucleation/growth and Li volume expansion during charging cause serious safety problems for Li anode‐based batteries. Here the coating of nickel foam with graphitic carbon nitride (g‐C3N4) to have a 3D current collector (g‐C3N4@Ni foam) for dendrite‐free Li metal anodes is reported. The lithiophilic g‐C3N4 coupled with the 3D framework is demonstrated to be highly effective for promoting the uniform deposition of Li and suppressing the formation of dendrites. Both density functional theory calculations and experimental studies indicate the formation of a micro‐electric field resulting from the tri‐s‐triazine units of g‐C3N4, which induces numerous Li nuclei during the initial nucleation stage, effectively guiding the following Li growth on the 3D Ni foam to be well distributed. Furthermore, the 3D porous framework is favorable for absorbing any volume change and stabilizing the solid–electrolyte interphase layer during repeated Li plating/stripping. As such, a Li metal anode based on the g‐C3N4@Ni foam has a remarkable electrochemical performance with a high Coulombic efficiency (98% retention after 300 cycles), an ultralong lifespan up to 900 h, as well as a low overpotential (<15 mV at 1.0 mA cm?2) at a Li deposition of 9.0 mA h cm?2.  相似文献   

20.
A facile two‐step strategy is developed to design the large‐scale synthesis of hierarchical, unique porous architecture of ternary metal hydroxide nanowires grown on porous 3D Ni foam and subsequent effective sulfurization. The hierarchical Zn–Co–S nanowires (NWs) arrays are directly employed as an electrode for supercapacitors application. The as‐synthesized Zn–Co–S NWs deliver an ultrahigh areal capacity of 0.9 mA h cm?2 (specific capacity of 366.7 mA h g?1) at a current density of 3 mA cm?2, with an exceptional rate capability (≈227.6 mA h g?1 at a very high current density of 40 mA cm?2) and outstanding cycling stability (≈93.2% of capacity retention after 10 000 cycles). Most significantly, the assembled Zn–Co–S NWs//Fe2O3@reduced graphene oxide asymmetric supercapacitors with a wide operating potential window of ≈1.6 V yield an ultrahigh volumetric capacity of ≈1.98 mA h cm?3 at a current density of 3 mA cm?2, excellent energy density of ≈81.6 W h kg?1 at a power density of ≈559.2 W kg?1, and exceptional cycling performance (≈92.1% of capacity retention after 10 000 cycles). This general strategy provides an alternative to design the other ternary metal sulfides, making it facile, free‐standing, binder‐free, and cost‐effective ternary metal sulfide‐based electrodes for large‐scale applications in modern electronics.  相似文献   

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