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1.
Although silicon‐based materials are ideal candidate anodes for high energy density lithium‐ion batteries, the large volumetric expansion seriously damages the integrity of the electrodes and impedes commercial processes. Reasonable electrode design based on adjustable structures of silicon and strong binders prepared by a facile method is still a great challenge. Herein, a three‐pronged collaborative strategy via hollow nanocubes, amorphous Void@SiOx@C, and in situ cross‐linked polyacrylic acid and d ‐sorbitol 3D network binder (c‐PAA‐DS) is adopted to maintain structural/electrode integrality and stability. The all‐integrated c‐PAA‐DS/Void@SiOx@C electrode delivers excellent mechanical property, which is attributed to ductility of the c‐PAA‐DS binder and high adhesion energy between Void@SiOx@C and c‐PAA‐DS calculated by density functional theory. Benefiting from the synergistic effect of accommodation of the hollow structure, protection of outer carbon shell, amorphous Void@SiOx@C, and strong adhesive c‐PAA‐DS binder, c‐PAA‐DS/Void@SiOx@C shows excellent electrochemical performance. Long cycling stability with a reversible capacity of 696 mAh g?1 is obtained, as well as tiny capacity decay after 500 cycles at 0.5 A g?1 and high‐rate performance. The prelithiated Void@SiOx@C||LiNi0.5Co0.2Mn0.3O2 (NCM523) full cell is also assembled and shows a reversible capacity of 157 mAh g?1 at 0.5 C, delivering an excellent capacity retention of 94% after 160 cycles.  相似文献   

2.
Here a simple and an environmentally friendly approach is developed for the fabrication of Si–void@SiOx nanowires of a high‐capacity Li‐ion anode material. The outer surface of the robust SiOx backbone and the inside void structure in Si–void@SiOx nanowires appropriately suppress the volume expansion and lead to anisotropic swelling morphologies of Si nanowires during lithiation/delithiation, which is first demonstrated by the in situ lithiation process. Remarkably, the Si–void@SiOx nanowire electrode exhibits excellent overall lithium‐storage performance, including high specific capacity, high rate property, and excellent cycling stability. A reversible capacity of 1981 mAh g?1 is obtained in the fourth cycle, and the capacity is maintained at 2197 mAh g?1 after 200 cycles at a current density of 0.5 C. The outstanding overall properties of the Si–void@SiOx nanowire composite make it a promising anode material of lithium‐ion batteries for the power‐intensive energy storage applications.  相似文献   

3.
A binder‐free efficient MoNi4/MoO3‐x nanorod array electrode with 3D open structure is developed by using Ni foam as both scaffold and Ni source to form NiMoO4 precursor, followed by subsequent annealing in a reduction atmosphere. It is discovered that the self‐templated conversion of NiMoO4 into MoNi4 nanocrystals and MoO3‐x as dual active components dramatically boosts the hydrogen evolution reaction (HER) performance. Benefiting from high intrinsic activity, high electrochemical surface area, 3D open network, and improved electron transport, the resulting MoNi4/MoO3‐x electrode exhibits a remarkable HER activity with extremely low overpotentials of 17 mV at 10 mA cm?2 and 114 mV at 500 mA cm?2, as well as a superior durability in alkaline medium. The water–alkali electrolyzer using MoNi4/MoO3‐x as cathode achieves stable overall water splitting with a small cell voltage of 1.6 V at 30 mA cm ? 2. These findings may inspire the exploration of cost‐effective and efficient electrodes by in situ integrating multiple highly active components on 3D platform with open conductive network for practical hydrogen production.  相似文献   

4.
A novel uniform amorphous carbon‐coated SnO2 nanocrystal (NCs) for use in lithium‐ion batteries is formed by utilizing bovine serum albumin (BSA) as both the ligand and carbon source. The SnO2–carbon composite is then coated by a controlled thickness of polydopamine (PD) layer through in situ polymerization of dopamine. The PD‐coated SnO2–carbon composite is finally mixed with polyacrylic acid (PAA) which is used as binder to accomplish a whole anode system. A crosslink reaction is built between PAA and PD through formation of amide bonds to produce a robust network in the anode system. As a result, the designed electrode exhibits improved reversible capacity of 648 mAh/g at a current density of 100 mA/g after 100 cycles, and an enhanced rate performance of 875, 745, 639, and 523 mAh/g at current densities of 50, 100, 250, and 500 mA/g, respectively. FTIR spectra confirm the formation of crosslink reaction and the stability of the robust network during long‐term cycling. The great improvement of capacity and rate performance achieved in this anode system is attributed to two stable interfaces built between the active material (SnO2–carbon composite) and the buffer layer (PD) and between the buffer layer and the binder (PAA), which effectively diminish the volume change of SnO2 during charge/discharge process and provide a stable matrix for active materials.  相似文献   

5.
Freestanding bifunctional electrodes with outstanding oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) properties are of great significance for zinc–air batteries, attributed to the avoided use of organic binder and strong adhesion with substrates. Herein, a strategy is developed to fabricate freestanding bifunctional electrodes from the predeposited nickel nanoparticles (Ni‐NCNT) on carbon fiber paper. The steric effect of monodispersed SiO2 nanospheres limits the configuration of carbon atoms forming 3D interconnected nanotubes with uniformly distributed NiN2 active sites. The bifunctional electrodes (Ni‐NCNT) demonstrate ideal ORR and OER properties. The zinc–air batteries assembled with Ni‐NCNT directly exhibit extremely outstanding long term stability (2250 cycles with 10 mA cm?2 charge/discharge current density) along with high power density of 120 mV cm?2 and specific capacity of 834.1 mA h g?1. This work provides a new view to optimize the distribution of active sites and the electrode structure.  相似文献   

6.
The development of cost‐effective and flexible electrodes is demanding in the field of energy storage. Herein, flexible FexOy/nitrogen‐doped carbon films (FexOy/NC‐MOG) are prepared by facile electrospinning of Fe‐based metal–organic gels (MOGs) followed by high‐temperature carbonization. This approach allows the even mixing of fragile coordination polymers with polyacrylonitrile into flexible films while reserving the structural characteristics of coordination polymers. After thermal treatment, FexOy/NC‐MOG films possess uniformly distributed FexOy nanoparticles and larger accessible surface areas than traditional FexOy‐NC films without MOG. Taking advantage of the unique structure, FexOy/NC‐MOG exhibits a superior rate performance (449.8 mA h g?1 at 5000 mA g–1) and long cycle life (629.3 mA h g–1 after 500 cycles at 1000 mA g–1) when used as additive‐free anodes in lithium‐ion batteries.  相似文献   

7.
Rational design and synthesis of hetero‐coordinated moieties at the atomic scale can significantly raise the performance of the catalyst and obtain mechanistic insight into the oxygen‐involving electrocatalysis. Here, a facile plasma‐photochemical strategy is applied to construct atomically coordinated Pt–Co–Se moieties in defective CoSe2 (CoSe2?x) through filling the plasma‐created Se vacancies in CoSe2?x with single Pt atomic species (CoSe2?x‐Pt) under ultraviolet irradiation. The filling of single Pt can remarkably enhance the oxygen evolution reaction (OER) activity of CoSe2. Optimal OER specific activity is achieved with a Pt content of 2.25 wt% in CoSe2?x‐Pt, exceeding that of CoSe2?x by a factor of 9. CoSe2?x‐Pt shows much better OER performance than CoSe2?x filled with single Ni and even Ru atomic species (CoSe2?x‐Ni and CoSe2?x‐Ru). Noticeably, it is general that Pt is not a good OER catalyst but Ru is; thus the design of active sites for electrocatalysis at an atomic level should follow a different intrinsic mechanism. Mechanism studies unravel that the single Pt can induce much higher electronic distribution asymmetry degree than both single Ni and Ru, and benefit the interaction between the Co sites and adsorbates (OH*, O*, and OOH*) during the OER process, leading to a better OER activity.  相似文献   

8.
Fabrication of hierarchical nanosheet arrays of 1T phase of transition‐metal dichalcogenides is indeed a critical task, but it holds immense potential for energy storage. A single‐step strategy is employed for the fabrication of stable 1T‐MnxMo1–xS2–ySey and MoFe2S4–zSez hierarchical nanosheet arrays on carbon cloth as positive and negative electrodes, respectively. The flexible asymmetric supercapacitor constructed with these two electrodes exhibits an excellent electrochemical performance (energy density of ≈69 Wh kg?1 at a power density of 0.985 kW kg?1) with ultralong cyclic stability of ≈83.5% capacity retention, after 10 000 consecutive cycles. Co‐doping of the metal and nonmetal boosts the charge storage ability of the transition‐metal chalcogenides following enrichment in the metallic 1T phase, improvement in the surface area, and expansion in the interlayer spacing in tandem, which is the key focus of the present study. This study explicitly demonstrates the exponential enhancement of specific capacity of MoS2 following intercalation and doping of Mn and Se, and Fe2S3 following doping of Mo and Se could be an ideal direction for the fabrication of novel energy‐storage materials with high‐energy storage ability.  相似文献   

9.
The CuS(x wt%)@Cu‐BTC (BTC = 1,3,5‐benzenetricarboxylate; x = 3, 10, 33, 58, 70, 99.9) materials are synthesized by a facile sulfidation reaction. The composites are composed of octahedral Cu3(BTC)2·(H2O)3 (Cu‐BTC) with a large specific surface area and CuS with a high conductivity. The as‐prepared CuS@Cu‐BTC products are first applied as the anodes of lithium‐ion batteries (LIBs). The synergistic effect between Cu‐BTC and CuS components can not only accommodate the volume change and stress relaxation of electrodes but also facilitate the fast transport of Li ions. Thus, it can greatly suppress the transformation process from Li2S to polysulfides by improving the reversibility of the conversion reaction. Benefiting from the unique structural features, the optimal CuS(70 wt%)@Cu‐BTC sample exhibits a remarkably improved electrochemical performance, showing an over‐theoretical capacity up to 1609 mAh g?1 after 200 cycles (100 mA g?1) with an excellent rate‐capability of ≈490 mAh g?1 at 1000 mA g?1. The outstanding LIB properties indicate that the CuS(70 wt%)@Cu‐BTC sample is a highly desirable electrode material candidate for high‐performance LIBs.  相似文献   

10.
A major obstacle for the use of single‐wall carbon nanotubes (SWCNTs) in electronic devices is their mixture of different types of electrical conductivity that strongly depends on their helical structure. The existence of metal impurities as a residue of a metallic growth catalyst may also lower the performance of SWCNT‐based devices. Here, it is shown that by using silicon oxide (SiOx) nanoparticles as a catalyst, metal‐free semiconducting and metallic SWCNTs can be selectively synthesized by the chemical vapor deposition of ethanol. It is found that control over the nanoparticle size and the content of oxygen in the SiOx catalyst plays a key role in the selective growth of SWCNTs. Furthermore, by using the as‐grown semiconducting and metallic SWCNTs as the channel material and source/drain electrodes, respectively, all‐SWCNT thin‐film transistors are fabricated to demonstrate the remarkable potential of these SWCNTs for electronic devices.  相似文献   

11.
High‐performance solution‐processed metal oxide (MO) thin‐film transistors (TFTs) are realized by fabricating a homojunction of indium oxide (In2O3) and polyethylenimine (PEI)‐doped In2O3 (In2O3:x% PEI, x = 0.5–4.0 wt%) as the channel layer. A two‐dimensional electron gas (2DEG) is thereby achieved by creating a band offset between the In2O3 and PEI‐In2O3 via work function tuning of the In2O3:x% PEI, from 4.00 to 3.62 eV as the PEI content is increased from 0.0 (pristine In2O3) to 4.0 wt%, respectively. The resulting devices achieve electron mobilities greater than 10 cm2 V?1 s?1 on a 300 nm SiO2 gate dielectric. Importantly, these metrics exceed those of the devices composed of the pristine In2O3 materials, which achieve a maximum mobility of ≈4 cm2 V?1 s?1. Furthermore, a mobility as high as 30 cm2 V?1 s?1 is achieved on a high‐k ZrO2 dielectric in the homojunction devices. This is the first demonstration of 2DEG‐based homojunction oxide TFTs via band offset achieved by simple polymer doping of the same MO material.  相似文献   

12.
Ammonia synthesis is one of the most kinetically complex and energetically challenging chemical processes in industry and has used the Harber–Bosch catalyst for over a century, which is processed under both harsh pressure (150–350 atm) and hightemperature (623–823 K), wherein the energy and capital intensive Harber–Bosch process has a huge energy cost accounting for about 1%–3% of human's energy consumption. Therefore, there has been a rough and vigorous exploration to find an environmentally benign alternative process. As the amorphous material is in a metastable state and has many “dangling bonds”, it is more active than the crystallized one. In this paper, CeOx ‐induced amorphization of Au nanoparticles anchored on reduced graphite oxide (a‐Au/CeOx –RGO) has been achieved by a facile coreduction method under ambient atmosphere. As a proof‐of‐concept experiment, a‐Au/CeOx –RGO hybrid catalyst containing the low noble metal (Au loading is 1.31 wt%) achieves a high Faradaic efficiency (10.10%) and ammonia yield (8.3 μg h?1 mg?1cat.) at ?0.2 V versus RHE, which is significantly higher than that of the crystalline counterpart (c‐Au/RGO), and even comparable to the yields and efficiencies under harsh temperatures and/or pressures.  相似文献   

13.
The recently emerging metal–air batteries equipped with advanced oxygen electrodes have provided enormous opportunities to develop the next generation of wearable and bio‐adaptable power sources. Theoretically, neutral electrolyte‐based Mg–air batteries possess potential advantages in electronics and biomedical applications over the other metal–air counterparts, especially the alkaline‐based Zn–air batteries. However, the rational design of advanced oxygen electrode for Mg–air batteries with high discharge voltage and capacity under neutral conditions still remains a major challenge. Inspired by fibrous string structures of bufo‐spawn, it is reported here that the scalable synthesis of atomic Fe–Nx coupled open‐mesoporous N‐doped‐carbon nanofibers (OM‐NCNF‐FeNx) as advanced oxygen electrode for Mg–air batteries. The fabricated OM‐NCNF‐FeNx electrodes present manifold advantages, including open‐mesoporous and interconnected structures, 3D hierarchically porous networks, good bio‐adaptability, homogeneously coupled atomic Fe–Nx sites, and high oxygen electrocatalytic performances. Most importantly, the assembled Mg–air batteries with neutral electrolytes reveal high open‐circuit voltage, stable discharge voltage plateaus, high capacity, long operating life, and good flexibility. Overall, the discovery on fabricating atomic OM‐NCNF‐FeNx electrode will not only create new pathways for achieving flexible, wearable, and bio‐adaptable power sources, but also take a step towards the scale‐up production of advanced nanofibrous carbon electrodes for a broad range of applications.  相似文献   

14.
Novel structured composite microspheres of metal oxide and nitrogen‐doped graphitic carbon (NGC) have been developed as efficient anode materials for lithium‐ion batteries. A new strategy is first applied to a one‐pot preparation of composite (FeOx‐NGC/Y) microspheres via spray pyrolysis. The FeOx‐NGC/Y composite microspheres have a yolk–shell structure based on the iron oxide material. The void space of the yolk–shell microsphere is filled with NGC. Dicyandiamide additive plays a key role in the formation of the FeOx‐NGC/Y composite microspheres by inducing Ostwald ripening to form a yolk–shell structure based on the iron oxide material. The FeOx‐NGC/Y composite microspheres with the mixed crystal structure of rock salt FeO and spinel Fe3O4 phases show highly superior lithium‐ion storage performances compared to the dense‐structured FeOx microspheres with and without carbon material. The discharge capacities of the FeOx‐NGC/Y microspheres for the 1st and 1000th cycle at 1 A g?1 are 1423 and 1071 mAh g?1, respectively. The microspheres have a reversible discharge capacity of 598 mAh g?1 at an extremely high current density of 10 A g?1. Furthermore, the strategy described in this study is generally applied to multicomponent metal oxide–carbon composite microspheres with yolk–shell structures based on metal oxide materials.  相似文献   

15.
SnOx (x = 0, 1, 2) and TiO2 are widely considered to be potential anode candidates for next generation lithium ion batteries. In terms of the lithium storage mechanisms, TiO2 anodes operate on the base of the Li ion intercalation–deintercalation, and they typically display long cycling life and high rate capability, arising from the negligible cell volume change during the discharge–charge process, while their performance is limited by low specific capacity and low electronic conductivity. SnOx anodes rely on the alloying–dealloying reaction with Li ions, and typically exhibit large specific capacity but poor cycling performance, originating from the extremely large volume change and thus the resultant pulverization problems. Making use of their advantages and minimizing the disadvantages, numerous strategies have been developed in the recent years to design composite nanostructured Sn–Ti–O ternary systems. This Review aims to provide rational understanding on their design and the improvement of electrochemical properties of such systems, including SnOx–TiO2 nanocomposites mixing at nanoscale and nanostructured SnxTi1‐xO2 solid solutions doped at the atomic level, as well as their combinations with carbon‐based nanomaterials.  相似文献   

16.
Polyamide 6 (PA6) based nanocomposites reinforced with 1–7 wt% silicon carbide nanoparticles (SiCp) and toughened with 20 wt% maleated styrene–ethylene–butylene–
stryrene (SEBS‐g‐MA) were fabricated by melt blending followed by injection moulding. The effects of SiCp addition on thermal and mechanical properties of such nanocomposites were investigated. Differential scanning calorimetry tests showed that SiCp act as effective nucleators for the crystallization of PA6 and enhance the degree of crystallinity. Mechanical measurements revealed that SiCp addition improves the Young's modulus and yield strength of PA6/SEBS‐g‐MA 80/20 blend at the expenses of tensile ductility and impact strength. The essential work of fracture (EWF) approach under tensile mode was employed to characterize the fracture toughness of PA6/SEBS‐g‐MA/SiCp nanocomposites. EWF results indicated that SiCp addition reduces both the specific EWF and specific non‐essential plastic work of fracture. Thus SiCp additions were detrimental to the fracture toughness of PA6/SEBS‐g‐MA 80/20 blends.  相似文献   

17.
SiOx is proposed as one of the most promising anodes for Li‐ion batteries (LIBs) for its advantageous capacity and stable Li uptake/release electrochemistry, yet its practical application is still a big challenge. Here encapsulation of SiOx nanoparticles into conductive graphene bubble film via a facile and scalable self‐assembly in solution is shown. The SiOx nanoparticles are closely wrapped in multilayered graphene to reconstruct a flake‐graphite‐like macrostructure, which promises uniform and agglomeration‐free distribution of SiOx in the carbon while ensures a high mechanical strength and a high tap density of the composite. The composites present unprecedented cycling stability and excellent rate capabilities upon Li storage, rendering an opportunity for its anode use in the next‐generation high‐energy LIBs.  相似文献   

18.
Nanosized WC, and binders Co, Ti and Ti‐Co, are used to process hardmetals. Titanium (Ti) was proposed to reduce and even replace the Co in these composites, verifying the effectiveness of the new binders. Samples of nanosized WC with 10 wt% Co, 9 wt% WC 1 wt% Ti – Co, WC‐10 wt% Ti were cold compacted at 200 MPa and sintered at 1500°C during 1 hour under vacuum of 10–2 mbar for the processing of hardmetal were performed. The structural characterization by X‐ray diffraction and microstructure by scanning electron microscopy (SEM) and EDS microanalysis of the sintered material. We observed the presence of the W2C phase in the sintered samples, and Co3W phases in the samples with Co content and a good distribution of binder phase, leading to formation of small “pool” of Co and Ti and small porosity and well distributed. It was proved that using Ti as binder phase, the neta phase formation was avoided.  相似文献   

19.
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   

20.
High‐performance of lithium‐ion batteries (LIBs) rely largely on the scrupulous design of nanoarchitectures and smart hybridization of bespoke active materials. In this work, the pine‐needle‐like Cu–Co skeleton is reported to support highly active Li4Ti5O12 (LTO) forming Cu–Co/LTO core–branch arrays via a united hydrothermal‐atomic layer deposition (ALD) method. ALD‐formed LTO layer is uniformly anchored on the pine‐needle‐like heterostructured Cu–Co backbone, which consists of branched Co nanowires (diameters in 20 nm) and Cu nanowires (250–300 nm) core. The designed Cu–Co/LTO core–branch arrays show combined advantages of large porosity, high electrical conductivity, and good adhesion. Due to the unique positive features, the Cu–Co/LTO electrodes are demonstrated with enhanced electrochemical performance including excellent high‐rate capacity (155 mAh g?1 at 20 C) and noticeable long‐term cycles (144 mAh g?1 at 20 C after 3000 cycles). Additionally, the full cell assembled with activated carbon positive electrode and Cu–Co/LTO negative electrode exhibits high power/energy densities (41.6 Wh kg?1 at 7.5 kW kg?1). The design protocol combining binder‐free characteristics and array configuration opens a new door for construction of advanced electrodes for application in high‐rate electrochemical energy storage.  相似文献   

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