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1.
A facile one‐step spraying synthesis of MoS2/C microspheres and their enhanced electrochemical performance as anode of sodium‐ion batteries is reported. An aerosol spraying pyrolysis without any template is employed to synthesize MoS2/C microspheres, in which ultrathin MoS2 nanosheets (≈2 nm) with enlarged interlayers (≈0.64 nm) are homogeneously embedded in mesoporous carbon microspheres. The as‐synthesized mesoporous MoS2/C microspheres with 31 wt% carbon have been applied as an anode material for sodium ion batteries, demonstrating long cycling stability (390 mAh g?1 after 2500 cycles at 1.0 A g?1) and high rate capability (312 mAh g?1 at 10.0 A g?1 and 244 mAh g?1 at 20.0 A g?1). The superior electrochemical performance is due to the uniform distribution of ultrathin MoS2 nanosheets in mesoporous carbon frameworks. This kind of structure not only effectively improves the electronic and ionic transport through MoS2/C microspheres, but also minimizes the influence of pulverization and aggregation of MoS2 nanosheets during repeated sodiation and desodiation.  相似文献   

2.
Nonmetallic plasmonic heterostructure TiO2‐mesocrystals/WO3?x‐nanowires (TiO2‐MCs/WO3?x‐NWs) are constructed by coupling mesoporous crystal TiO2 and plasmonic WO3?x through a solvothermal procedure. The continuous photoelectron injection from TiO2 stabilizes the free carrier density and leads to strong surface plasmon resonance (SPR) of WO3?x, resulting in strong light absorption in the visible and near‐infrared region. Photocatalytic hydrogen generation of TiO2‐MCs/WO3?x‐NWs is attributed to plasmonic hot electrons excited on WO3?x‐NWs under visible light irradiation. However, utilization of injected photoelectrons on WO3?x‐NWs has low efficiency for hydrogen generation and a co‐catalyst (Pt) is necessary. TiO2‐MCs/WO3?x‐NWs are used as co‐catalyst free plasmonic photocatalysts for CO2 reduction, which exhibit much higher activity (16.3 µmol g?1 h?1) and selectivity (83%) than TiO2‐MCs (3.5 µmol g?1 h?1, 42%) and WO3?x‐NWs (8.0 µmol g?1 h?1, 64%) for methane generation under UV–vis light irradiation. A photoluminescence study demonstrates the photoelectron injection from TiO2 to WO3?x, and the nonmetallic SPR of WO3?x plays a great role in the highly selective methane generation during CO2 photoreduction.  相似文献   

3.
Photocatalytic H2O2 evolution through two‐electron oxygen reduction has attracted wide attention as an environmentally friendly strategy compared with the traditional anthraquinone or electrocatalytic method. Herein, a biomimetic leaf‐vein‐like g‐C3N4 as an efficient photocatalyst for H2O2 evolution is reported, which owns tenable band structure, optimized charge transfer, and selective two‐electron O2 reduction. The mechanism for the regulation of band structure and charge transfer is well studied by combining experiments and theoretical calculations. The H2O2 yield of CN4 (287 µmol h?1) is about 3.3 times higher than that of pristine CN (87 µmol h?1), and the apparent quantum yield for H2O2 evolution over CN4 reaches 27.8% at 420 nm, which is much higher than that for many other current photocatalysts. This work not only provides a novel strategy for the design of photocatalyst with excellent H2O2 evolution efficiency, but also promotes deep understanding for the role of defect and doping sites on photocatalytic activity.  相似文献   

4.
A 2D/2D heterojunction of black phosphorous (BP)/graphitic carbon nitride (g‐C3N4) is designed and synthesized for photocatalytic H2 evolution. The ice‐assisted exfoliation method developed herein for preparing BP nanosheets from bulk BP, leads to high yield of few‐layer BP nanosheets (≈6 layers on average) with large lateral size at reduced duration and power for liquid exfoliation. The combination of BP with g‐C3N4 protects BP from oxidation and contributes to enhanced activity both under λ > 420 nm and λ > 475 nm light irradiation and to long‐term stability. The H2 production rate of BP/g‐C3N4 (384.17 µmol g?1 h?1) is comparable to, and even surpasses that of the previously reported, precious metal‐loaded photocatalyst under λ > 420 nm light. The efficient charge transfer between BP and g‐C3N4 (likely due to formed N? P bonds) and broadened photon absorption (supported both experimentally and theoretically) contribute to the excellent photocatalytic performance. The possible mechanisms of H2 evolution under various forms of light irradiation is unveiled. This work presents a novel, facile method to prepare 2D nanomaterials and provides a successful paradigm for the design of metal‐free photocatalysts with improved charge‐carrier dynamics for renewable energy conversion.  相似文献   

5.
This study reports the design and fabrication of ultrathin MoS2 nanosheets@metal organic framework‐derived N‐doped carbon nanowall array hybrids on flexible carbon cloth (CC@CN@MoS2) as a free‐standing anode for high‐performance sodium ion batteries. When evaluated as an anode for sodium ion battery, the as‐fabricated CC@CN@MoS2 electrode exhibits a high capacity (653.9 mA h g?1 of the second cycle and 619.2 mA h g?1 after 100 cycles at 200 mA g?1), excellent rate capability, and long cycling life stability (265 mA h g?1 at 1 A g?1 after 1000 cycles). The excellent electrochemical performance can be attributed to the unique 2D hybrid structures, in which the ultrathin MoS2 nanosheets with expanded interlayers can provide shortened ion diffusion paths and favorable Na+ insertion/extraction space, and the porous N‐doped carbon nanowall arrays on flexible carbon cloth are able to improve the conductivity and maintain the structural integrity. Moreover, the N‐doping‐induced defects also make them favorable for the effective storage of sodium ions, which enables the enhanced capacity and rate performance of MoS2.  相似文献   

6.
Flexible freestanding electrodes are highly desired to realize wearable/flexible batteries as required for the design and production of flexible electronic devices. Here, the excellent electrochemical performance and inherent flexibility of atomically thin 2D MoS2 along with the self‐assembly properties of liquid crystalline graphene oxide (LCGO) dispersion are exploited to fabricate a porous anode for high‐performance lithium ion batteries. Flexible, free‐standing MoS2–reduced graphene oxide (MG) film with a 3D porous structure is fabricated via a facile spontaneous self‐assembly process and subsequent freeze‐drying. This is the first report of a one‐pot self‐assembly, gelation, and subsequent reduction of MoS2/LCGO composite to form a flexible, high performance electrode for charge storage. The gelation process occurs directly in the mixed dispersion of MoS2 and LCGO nanosheets at a low temperature (70 °C) and normal atmosphere (1 atm). The MG film with 75 wt% of MoS2 exhibits a high reversible capacity of 800 mAh g?1 at a current density of 100 mA g?1. It also demonstrates excellent rate capability, and excellent cycling stability with no capacity drop over 500 charge/discharge cycles at a current density of 400 mA g?1.  相似文献   

7.
The large volume expansion induced by K+ intercalation is always a big challenge for designing high‐performance electrode materials in potassium‐ion storage system. Based on the idea that large‐sized ions should accommodate big “houses,” a facile‐induced growth strategy is proposed to achieve the self‐loading of MoS2 clusters inside a hollow tubular carbon skeleton (HTCS). Meantime, a step‐by‐step intercalation technology is employed to tune the interlayer distance and the layer number of MoS2. Based on the above, the ED‐MoS2@CT hybrids are achieved by self‐loading and anchoring the well‐dispersed ultrathin MoS2 nanosheets on the inner surface of HTCSs. This unique compositing model not only alleviates the mechanical strain efficiently, but also provides spacious “roads” (hollow tubular carbon skeleton) and “houses” (interlayer expanded ultrathin MoS2 sheets) for fast K+ transition and storage. As an anode of potassium‐ion batteries, the resultant ED‐MoS2@CT electrode delivers a high specific capacity of 148.5 mAh g?1 at 2 A g?1 after 10 000 cycles with only 0.002% fading per cycle. The assembled ED‐MoS2@CT//PC potassium‐ion hybrid supercapacitor device shows a high energy density of 148 Wh kg?1 at a power density of 965 W kg?1, which is comparable to that of lithium‐ion hybrid supercapacitors.  相似文献   

8.
Exploring a universal strategy to implement the precise control of 2D nanomaterials in size and layer number is a big challenge for achieving ultrafast and stable Li/Na‐ion batteries. Herein, the confined synthesis of 1–3 layered MoS2 nanocrystals into 2D Ti3C2 interlayer nanospace with the help of electrostatic attraction and subsequent cetyltrimethyl ammonium bromide (CTAB) directed growth is reported. The MoS2 nanocrystals are tightly anchored into the interlayer by 2D confinement effect and strong Mo? C covalent bond. Impressively, the disappearance of Li+ intercalated into MoS2 reduction peak is successfully observed for the first time in the experiment, showing in a typical surface‐controlled charge storage behavior. The pseudocapacitance‐dominated contribution guarantees a much faster and more stable Li/Na storage performance. As predicted, this electrode exhibits a very high Li+ storage capacity of 340 mAh g?1 even at 20 A g?1 and a long cycle life (>1000 times). It also shows an excellent Na+ storage capacity of 310 mAh g?1 at 1 A g?1 with a 1600 times high‐rate cycling. Such impressive confined synthesis strategy can be extended to the precise control of other 2D nanomaterials.  相似文献   

9.
Dark‐colored rutile TiO2 nanorods doped by electroconducting Ti3+ have been obtained uniformly with an average diameter of ≈7 nm, and have been first utilized as anodes in lithium‐ion batteries. They deliver a high reversible specific capacity of 185.7 mAh g?1 at 0.2 C (33.6 mA g?1) and maintain 92.1 mAh g?1 after 1000 cycles at an extremely high rate 50 C with an outstanding retention of 98.4%. Notably, the coulombic efficiency of Ti3+–TiO2 has been improved by approximately 10% compared with that of pristine rutile TiO2, which can be mainly attributed to its prompt electron transfer because of the introduction of Ti3+. Again the synergetic merits are noticed when the promoted electronic conductivity is combined with a shortened Li+ diffusion length resulting from the ultrafine nanorod structure, giving rise to the remarkable rate capabilities and extraordinary cycling stabilities for applications in fast and durable charge/discharge batteries. It is of great significance to incorporate Ti3+ into rutile TiO2 to exhibit particular electrochemical characteristics triggering an effective way to improve the energy storage properties.  相似文献   

10.
Anisotropic Ag2S‐edged Au‐triangular nanoprisms (TNPs) are constructed by controlling preferential overgrowth of Ag2S as plasmonic photocatalysts for hydrogen generation. Under visible and near‐infrared light irradiation, Ag2S‐edged Au‐TNPs exhibit almost fourfold higher efficiency (796 µmol h−1 g−1) than those of Ag2S‐covered Au‐TNPs (216 µmol h−1 g−1) and pure Au‐TNPs in hydrogen generation. A single‐particle photoluminescence study demonstrates that the plasmon‐induced hot electrons transfer from Au‐TNPs to Ag2S for hydrogen generation. Finite‐difference‐time‐domain simulations verify that the corners/edges of Au‐TNPs are high‐curvature sites with maximum electric field distributions facilitating hot electron generation and transfer. Therefore, Ag2S‐edged Au‐TNPs are efficient plasmonic photocatalyst with the desired configurations for charge separation boosting hydrogen generation.  相似文献   

11.
Na‐ion Batteries have been considered as promising alternatives to Li‐ion batteries due to the natural abundance of sodium resources. Searching for high‐performance anode materials currently becomes a hot topic and also a great challenge for developing Na‐ion batteries. In this work, a novel hybrid anode is synthesized consisting of ultrafine, few‐layered SnS2 anchored on few‐layered reduced graphene oxide (rGO) by a facile solvothermal route. The SnS2/rGO hybrid exhibits a high capacity, ultralong cycle life, and superior rate capability. The hybrid can deliver a high charge capacity of 649 mAh g?1 at 100 mA g?1. At 800 mA g?1 (1.8 C), it can yield an initial charge capacity of 469 mAh g?1, which can be maintained at 89% and 61%, respectively, after 400 and 1000 cycles. The hybrid can also sustain a current density up to 12.8 A g?1 (≈28 C) where the charge process can be completed in only 1.3 min while still delivering a charge capacity of 337 mAh g?1. The fast and stable Na‐storage ability of SnS2/rGO makes it a promising anode for Na‐ion batteries.  相似文献   

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

13.
Using synergetic effects of various sodium storage modes and materials to construct high power, high energy, and long cycling flexible sodium anode materials is significant and still challenging. Here, by advantageous functional integration of adsorption‐intercalation‐conversion sodium storage mechanisms, a 3D flexible fiber paper anode with the composition of Nb2O5@hard carbon@MoS2@soft carbon is designed and prepared. Based on the synergetic effects, it exhibits higher specific capacity than pure Nb2O5, with more excellent rate performance (245, 201, 155, 133, and 97 mAh g?1 at the current density of 0.2, 1, 5, 10, and 20 A g?1, respectively) than pure MoS2 as well as admirable long‐term cycling characteristics (≈82% capacity retention after 20 000 cycles at 5 A g?1). Relevant kinetics mechanisms are expounded in detail. This work can be helpful for preparing other types of hybrid and flexible electrodes for energy storage systems.  相似文献   

14.
Developing high‐efficiency and low‐cost photocatalysts by avoiding expensive noble metals, yet remarkably improving H2 evolution performance, is a great challenge. Noble‐metal‐free catalysts containing Co(Fe)?N?C moieties have been widely reported in recent years for electrochemical oxygen reduction reaction and have also gained noticeable interest for organic transformation. However, to date, no prior studies are available in the literature about the activity of N‐coordinated metal centers for photocatalytic H2 evolution. Herein, a new photocatalyst containing g‐C3N4 decorated with CoP nanodots constructed from low‐cost precursors is reported. It is for the first time revealed that the unique P(δ?)?Co(δ+)?N(δ?) surface bonding states lead to much superior H2 evolution activity (96.2 µmol h?1) compared to noble metal (Pt)‐decorated g‐C3N4 photocatalyst (32.3 µmol h?1). The quantum efficiency of 12.4% at 420 nm is also much higher than the record values (≈2%) of other transition metal cocatalysts‐loaded g‐C3N4. It is believed that this work marks an important step toward developing high‐performance and low‐cost photocatalytic materials for H2 evolution.  相似文献   

15.
Low‐power, nonvolatile memory is an essential electronic component to store and process the unprecedented data flood arising from the oncoming Internet of Things era. Molybdenum disulfide (MoS2) is a 2D material that is increasingly regarded as a promising semiconductor material in electronic device applications because of its unique physical characteristics. However, dielectric formation of an ultrathin low‐k tunneling on the dangling bond‐free surface of MoS2 is a challenging task. Here, MoS2‐based low‐power nonvolatile charge storage memory devices are reported with a poly(1,3,5‐trimethyl‐1,3,5‐trivinyl cyclotrisiloxane) (pV3D3) tunneling dielectric layer formed via a solvent‐free initiated chemical vapor deposition (iCVD) process. The surface‐growing polymerization and low‐temperature nature of the iCVD process enable the conformal growing of low‐k (≈2.2) pV3D3 insulating films on MoS2. The fabricated memory devices exhibit a tunable memory window with high on/off ratio (≈106), excellent retention times of 105 s with an extrapolated time of possibly years, and an excellent cycling endurance of more than 103 cycles, which are much higher than those reported previously for MoS2‐based memory devices. By leveraging the inherent flexibility of both MoS2 and polymer dielectric films, this research presents an important milestone in the development of low‐power flexible nonvolatile memory devices.  相似文献   

16.
Anatase TiO2 is considered as one of the promising anodes for sodium‐ion batteries because of its large sodium storage capacities with potentially low cost. However, the precise reaction mechanisms and the interplay between surface properties and electrochemical performance are still not elucidated. Using multimethod analyses, it is herein demonstrated that the TiO2 electrode undergoes amorphization during the first sodiation and the amorphous phase exhibits pseudocapacitive sodium storage behaviors in subsequent cycles. It is also shown that the pseudocapacitive sodium storage performance is sensitive to the nature of solid electrolyte interphase (SEI) layers. For the first time, it is found that ether‐based electrolytes enable the formation of thin (≈2.5 nm) and robust SEI layers, in contrast to the thick (≈10 nm) and growing SEI from conventional carbonate‐based electrolytes. First principle calculations suggest that the higher lowest unoccupied molecular orbital energies of ether solvents/ion complexes are responsible for the difference. TiO2 electrodes in ether‐based electrolyte present an impressive capacity of 192 mAh g?1 at 0.1 A g?1 after 500 cycles, much higher than that in carbonate‐based electrolyte. This work offers the clarified picture of electrochemical sodiation mechanisms of anatase TiO2 and guides on strategies about interfacial control for high performance anodes.  相似文献   

17.
Sodium‐ion batteries are widely considered as promising energy storage systems for large‐scale applications, but their relatively low energy density hinders further practical applications. Developing high‐voltage cathode materials is an effective approach to increase the overall energy density of sodium‐ion batteries. When cut‐off voltage is elevated over 4.3 V, however, the cathode becomes extremely unstable due to structural transformations as well as metal dissolution into the electrolytes. In this work, the cyclic stability of P2‐Na0.66(Mn0.54Co0.13Ni0.13)O2 (MCN) electrode at a cut‐off voltage of 4.5 V is successfully improved by using ultrathin metal oxide surface coatings (Al2O3, ZrO2, and TiO2) deposited by an atomic layer deposition technique. The MCN electrode coated with the Al2O3 layer exhibits higher capacity retention among the MCN electrodes. Moreover, the rate performance of the MCN electrode is greatly improved by the metal oxide coatings in the order of TiO2 < Al2O3 < ZrO2, due to increased fracture toughness and electrical conductivity of the metal oxide coating layers. A ZrO2‐coated MCN electrode shows a discharge capacity of 83 mAh g?1 at 2.4 A g?1, in comparison to 61 mAh g?1 for a pristine MCN electrode. Cyclic voltammetry and electrochemical impedance analysis disclose the reduced charge transfer resistance from 1421 to 760.2 Ω after cycles, suggesting that the metal oxide coating layer can effectively minimize the undesirable phase transition, buffer inherent stress and strain between the binder, cathode, and current collector, and avoid volumetric changes, thus increasing the cyclic stability of the MCN electrode.  相似文献   

18.
Room‐temperature sodium‐ion batteries have attracted great attentions for large‐scale energy storage applications in renewable energy. However, exploring suitable anode materials with high reversible capacity and cyclic stability is still a challenge. The VS4, with parallel quasi‐1D chains structure of V4+(S22?)2, which provides large interchain distance of 5.83 Å and high capacity, has showed great potential for sodium storage. Here, the uniform cuboid‐shaped VS4 nanoparticles are prepared as anode for sodium‐ion batteries by the controllable of graphene oxide (GO)‐template contents. It exhibits superb electrochemical performances of high‐specific charge capacity (≈580 mAh·g?1 at 0.1 A·g?1), long‐cycle‐life (≈98% retain at 0.5 A·g?1 after 300 cycles), and high rates (up to 20 A·g?1). In addition, electrolytes are optimized to understand the sodium storage mechanism. It is thus demonstrated that the findings have great potentials for the applications in high‐performance sodium‐ion batteries.  相似文献   

19.
Asymmetric Janus nanostructures containing a gold nanocage (NC) and a carbon–titania hybrid nanocrystal (AuNC/(C–TiO2)) are prepared using a novel and facile microemulsion‐based approach that involves the assistance of ethanol. The localized surface plasmon resonance of the Au NC with a hollow interior and porous walls induce broadband visible‐light harvesting in the Janus AuNC/(C–TiO2). An acetone evolution rate of 6.3 μmol h?1 g?1 is obtained when the Janus nanostructure is used for the photocatalytic aerobic oxidation of iso‐propanol under visible light (λ = 480–910 nm); the rate is 3.2 times the value of that obtained with C–TiO2, and in photo‐electrochemical investigations an approximately fivefold enhancement is obtained. Moreover, when compared with the core–shell structure (AuNC@(C–TiO2) and a gold–carbon–titania system where Au sphere nanoparticles act as light‐harvesting antenna, Janus AuNC/(C–TiO2) exhibit superior plasmonic enhancement. Electromagnetic field simulation and electron paramagnetic resonance results suggest that the plasmon–photon coupling effect is dramatically amplified at the interface between the Au NC and C–TiO2, leading to enhanced generation of energetic hot electrons for photocatalysis.  相似文献   

20.
This study is the first to demonstrate that ferroelectric R3c LiNbO3‐type ZnSnO3 nanowires (NWs), through the piezocatalysis and piezophototronic process, demonstrate a highly efficient hydrogen evolution reaction (HER). The polarization and electric field curves indicate that ZnSnO3 NWs exhibit typical ferroelectric hysteresis loops. Time‐resolved photoluminescence spectra reveal that the relaxation time increases with the increasing concentration of oxygen vacancies. Moderated 3H‐ZnSnO3 NWs (thermally annealed for 3 h in a hydrogen environment) have the longest extended carrier lifetime of approximately 8.3 ns. The piezoelectricity‐induced HER, via the piezocatalysis process (without light irradiation), reaches an optimal H2‐production rate of approximately 3453.1 µmol g?1 h?1. Through the synergistic piezophototronic process, the HER reaches approximately 6000 µmol g?1 in 7 h. Crucially, the mechanical force–induced spontaneous polarization functions as a carrier separator, driving the electron and hole in opposite directions in ferroelectric ZnSnO3 NWs; this separation reduces the recombination rate, enhancing the redox process. This theoretical analysis indicates that the photocatalytic and piezocatalytic effects can synergistically enhance piezophototronic performance through capitalizing on well‐modulated oxygen vacancies in ferroelectric semiconductors. This study demonstrates the essential role of this synergy in purifying water pollutants and converting water into hydrogen gas through the piezophototronic process.  相似文献   

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