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1.
Introducing inorganic fillers into organic poly(ethylene oxide)(PEO)-based electrolyte has attracted substantial attention to enhance its ionic conductivity and mechanical strength, but limited inorganic–organic interphases are always caused by isolated particles agglomeration. Herein, a variety of sandwich structured metal oxide/reduced graphene oxide(rGO)/metal oxide nanocomposites to optimize lithium-ion conduction by interconnected amorphous organic–inorganic interphases in lithium metal batteries, are proposed. With the support of high surface area rGO, the agglomeration of metal oxide particles is precluded, forming continuous amorphous organic–inorganic interphases with stacked layer-by-layer structure, thus creating 3D interconnected lithium-ion transportation channels vertically and laterally. Besides, metal oxide nanoparticles with hydroxyls possess high affinity toward bis(tri-fluoromethanesulfonyl)imide anions by hydrogen bindings between hydroxyls and fluorine and metal-oxygen bonds, releasing more free lithium ions. Consequently, PEO-ZnO/rGO/ZnO electrolyte delivers superior ionic conductivity of 1.02 × 10−4 S cm−1 at 25 °C and lithium-ion transference number of 0.38 at 60 °C. Furthermore, ZnO/rGO/ZnO insertion promotes the formation of LiF-rich stable solid electrolyte interface, endowing Li symmetric cells with long-term cycling stability over 900 hours. The corresponding LiFePO4 cathode possesses a high reversible specific capacity of 130 mAh g−1 at 0.5C after cycling 300 cycles with a poor capacity fading of 0.05% per cycle.  相似文献   

2.
The nature of the liquid–solid interface determines the characteristics of a variety of physical phenomena, including catalysis, electrochemistry, lubrication, and crystal growth. Most of the established models for crystal growth are based on macroscopic thermodynamics, neglecting the atomistic nature of the liquid–solid interface. Here, experimental observations and molecular dynamics simulations are employed to identify the 3D nature of an atomic-scale ordering of liquid Ga in contact with solid GaAs in a nanowire growth configuration. An interplay between the liquid ordering and the formation of a new bilayer is revealed, which, contrary to the established theories, suggests that the preference for a certain polarity and polytypism is influenced by the atomic structure of the interface. The conclusions of this work open new avenues for the understanding of crystal growth, as well as other processes and systems involving a liquid–solid interface.  相似文献   

3.
Among the alternatives to lithium-ion batteries, lithium–sulfur(Li–S)batteries are considered as an attractive option because of their high theoretical energy density of 2570 Wh kg-1. However, the application of the Li–S battery has been plagued by the rapid failure of the Li anode due to the Li dendrite growth and severe parasitic reactions between Li and lithium polysulfides. The physicochemical properties of the solid–electrolyte interphase have a profound impact on the performance...  相似文献   

4.
Materials enabling solar energy conversion and long-term storage for readily available electrical and chemical energy are key for off-grid energy distribution. Herein, the specific confinement of a rhenium coordination complex in a metal–organic framework (MOF) unlocks a unique electron accumulating property under visible-light irradiation. About 15 C gMOF−1 of electric charges can be concentrated and stored for over four weeks without loss. Decoupled, on-demand discharge for electrochemical reactions and H2 evolution catalysis is shown and light-driven recharging can be conducted for >10 cycles with ≈90% of the initial charging capacity retained. Experimental investigations and theoretical calculations link electron trapping to MOF-induced geometry constraints as well as the coordination environment of the Re-center, highlighting the key role of MOF confinement on molecular guests. This study serves as the seminal report on 3D porous colloids achieving photoaccumulation of long-lived electrons, unlocking dark photocatalysis, and a path toward solar capacitor and solar battery systems.  相似文献   

5.
Tremendous effort have recently been made in optimizing the air catalysts of flexible zinc–air batteries (ZABs). Unfortunately, the bottleneck factors in electrolytes that largely limit the working life and energy efficiency of ZABs have long been relatively neglected. Herein, an alkaline gel polymer electrolyte (GPE) is fabricated through multiple crosslinking reactions among poly(vinyl alcohol) (PVA), poly(acrylic acid), and graphene oxide followed by intense uptake of an alkali and the KI reaction modifier. The prepared GPE exhibits essentially improved properties compared to traditional PVA gel electrolyte in terms of mechanical strength, ionic conductivity, and water retention capability. In addition, the introduced reaction modifier I in the GPE changes the path of the conventional oxygen evolution reaction, leading to a more thermodynamically favorable path. The optimized GPE enables flexible ZABs exhibiting an exceptionally low charge potential of 1.69 V, a long cycling time of 200 h, a high energy efficiency of 73%, and rugged reliability under different extreme working conditions. Moreover, the successful integration of ZABs in a variety of real wearable electronic devices demonstrates their excellent practicability as flexible power sources.  相似文献   

6.
Umemoto  Yuki  Sugawara  Katsuaki  Nakata  Yuki  Takahashi  Takashi  Sato  Takafumi 《Nano Research》2019,12(1):165-169
Nano Research - One of important challenges in condensed-matter physics is to realize new quantum states of matter by manipulating the dimensionality of materials, as represented by the discovery...  相似文献   

7.
To study the temperature distribution and thermal-stress?eld in different service stages,a twodimensional model of a turbine blade with thermal barrier coatings is developed,in which the conjugate heat transfer analysis and the decoupled thermal-stress calculation method are adopted.Based on the simulation results,it is found that a non-uniform distribution of temperature appears in different positions of the blade surface,which has directly impacted on stress?eld.The maximum temperature with a value of 1030°C occurs at the leading edge.During the steady stage,the maximum stress of thermally grown oxide(TGO)appears in the middle of the suction side,reaching 3.75 GPa.At the end stage of cooling,the maximum compressive stress of TGO with a value of -3.5 GPa occurs at the leading edge.Thus,it can be predicted that during the steady stage the dangerous regions may locate at the suction side,while the leading edge may be more prone to failure on cooling.  相似文献   

8.
Three-dimensional (3D) reconfigurable patterns with dynamic morphologies enable the on-demand control of surface properties, such as optical, wetting, and adhesive properties, to achieve smart surfaces. Here, a simple yet general strategy is developed for fabricating 3D patterns with reversible wrinkles on the surface, in which a Diels–Alder (D-A) reaction in the top layer, which consists of a reversible cross-linked polymer network composed of a furan-containing copolymer (PSFB) and bismaleimide (BMI), can be spatially controlled by the photodimerization of BMI. When a photomask is used during irradiation with ultraviolet (UV) light, selective photodimerization of the maleimide leads to the diffusion of maleimide from the unexposed region to the exposed region, resulting in the generation of a diffused relief pattern. By controlling the reversible D-A reaction at different temperatures, orthogonal wrinkles can be sequentially and reversibly generated or erased in both the exposed and unexposed regions on the surface. Theoretical modeling with boundary effects reveals that the orientation of the wrinkle in the exposed region is perpendicular to the boundary, whereas the wrinkle in the unexposed region is parallel to the boundary. This strategy, based on a photocontrolled D-A reaction, provides an important and robust alternative for fabricating 3D patterned surfaces with dynamic topographies.  相似文献   

9.
Iron–cobalt alloy and cobalt–magnetite composites doped with Nd3+ (Co x Fe1?x /Co y Fe1?y Nd z Fe2?z O4) in which the Fe alloy has either a bcc or a fcc structure and the oxide is a spinel phase, have been synthesized by using the disproportionation of Fe(OH)2 and the reduction of Co(II) by Fe0 in a concentrated KOH solution. Powder X-ray diffraction, scanning electron microscope and vibrating sample magnetometer were employed to characterize the crystallite sizes, structure, morphology and magnetic properties of the composites. And the effect of the Co(II)/Fe(II) ratio (0 ≤ Co/Fe ≤ 1), concentration of KOH, reaction time and substitution Fe3+ ions by Nd3+ ions on structure, magnetic properties of the composites were investigated. From the perspective of thermodynamics, we explain the postulated mechanism of the disproportionation reaction.  相似文献   

10.
11.
This paper presents accurate numerical solutions for nonlinear eigenvalue analysis of three-dimensional acoustic cavities by boundary element method (BEM). To solve the nonlinear eigenvalue problem (NEP) formulated by BEM, we employ a contour integral method, called block Sakurai–Sugiura (SS) method, by which the NEP is converted to a standard linear eigenvalue problem and the dimension of eigenspace is reduced. The block version adopted in present work can also extract eigenvalues whose multiplicity is larger than one, but for the complex connected region which includes a internal closed boundary, the methodology yields fictitious eigenvalues. The application of the technique is demonstrated through the eigenvalue calculation of sphere with unique homogenous boundary conditions, cube with mixed boundary conditions and a complex connected region formed by cubic boundary and spherical boundary, however, the fictitious eigenvalues can be identified by Burton–Miller's method. These numerical results are supported by appropriate convergence study and comparisons with close form.  相似文献   

12.
The development of narrow-bandgap (Eg ≈ 1.2 eV) mixed tin–lead (Sn–Pb) halide perovskites enables all-perovskite tandem solar cells. Whereas pure-lead halide perovskite solar cells (PSCs) have advanced simultaneously in efficiency and stability, achieving this crucial combination remains a challenge in Sn–Pb PSCs. Here, Sn–Pb perovskite grains are anchored with ultrathin layered perovskites to overcome the efficiency-stability tradeoff. Defect passivation is achieved both on the perovskite film surface and at grain boundaries, an approach implemented by directly introducing phenethylammonium ligands in the antisolvent. This improves device operational stability and also avoids the excess formation of layered perovskites that would otherwise hinder charge transport. Sn–Pb PSCs with fill factors of 79% and a certified power conversion efficiency (PCE) of 18.95% are reported—among the highest for Sn–Pb PSCs. Using this approach, a 200-fold enhancement in device operating lifetime is achieved relative to the nonpassivated Sn–Pb PSCs under full AM1.5G illumination, and a 200 h diurnal operating time without efficiency drop is achieved under filtered AM1.5G illumination.  相似文献   

13.
14.
Heteroatom-doped transition metal-oxides of high oxygen evolution reaction (OER) activities interfaced with metals of low hydrogen adsorption energy barrier for efficient hydrogen evolution reaction (HER) when uniformly embedded in a conductive nitrogen-doped carbon (NC) matrix, can mitigate the low-conductivity and high-agglomeration of metal-nanoparticles in carbon matrix and enhances their bifunctional activities. Thus, a 3D mesoporous heterostructure of boron (B)-doped cobalt-oxide/cobalt-metal nanohybrids embedded in NC and grown on a Ni foam substrate (B-CoO/Co@NC/NF) is developed as a binder-free bifunctional electrocatalyst for alkaline water-splitting via a post-synthetic modification of the metal–organic framework and subsequent annealing in different Ar/H2 gas ratios. B-CoO/Co@NC/NF prepared using 10% H2 gas (B-CoO/Co@NC/NF [10% H2]) shows the lowest HER overpotential (196 mV) and B-CoO/Co@NC/NF (Ar), developed in Ar, shows an OER overpotential of 307 mV at 10 mA cm−2 with excellent long-term durability for 100 h. The best anode and cathode electrocatalyst-based electrolyzer (B-CoO/Co@NC/NF (Ar)(+)//B-CoO/Co@NC/NF (10% H2)(−)) generates a current density of 10 mA cm−2 with only 1.62 V with long-term stability. Further, density functional theory investigations demonstrate the effect of B-doping on electronic structure and reaction mechanism of the electrocatalysts for optimal interaction with reaction intermediates for efficient alkaline water-splitting which corroborates the experimental results.  相似文献   

15.
The Ti3AI matrix composite sheet with a novel quasi-continuous chain reinforcement distribution was prepared by using roll bonding and subsequent reaction annealing with pure Ti and SiCp/AI foils. The (Ti3AIC + TisSi3) reinforcements were produced by in situ reaction of the as-rolled Ti-(SiCp/AI) laminated composite sheet after a two-stage annealing treatment including first annealing at 660 °C and second annealing at 1250 °C. The microstructure evolution during the reaction annealing was investigated. In the first reaction annealing, TiAI3 was formed, and the SiC particles were pushed together due to the Kirkendall effect, and after the second reaction annealing, Ti3AI, Ti3AIC and Ti5Si3 were synthesized. In addition, the reinforcement distribution presents a quasi-continuous chain microstructure in Ti3AI matrix composite sheet.  相似文献   

16.
17.
Sub-micrometer Sc2O3–W powder with a narrow particle size distribution has been obtained by a sol–gel method combined with two-step hydrogen reduction process. Based on the obtained powder, the W–Sc2O3 targets have been sintered via spark plasma sintering (SPS) at 1300 °C. The W–Sc2O3 targets have the average grain size of about 1 μm. Both the sintering temperature and holding time are much lower than those of the targets prepared with micrometer sized powders. The obtained W–Sc2O3 targets have a high comparative density of 96.4% and rockwell hardness of 86.4 HRC. Using the target, the scandate cathode deposited with a film containing 5% Sc2O3 and 95% W has been obtained by pulsed laser deposition (PLD) method. This cathode has good emission property, i.e., the highest thermionic emission current density reaches 43.09 A/cm2 of Jdiv at 900 °Cb after being activated for 8 h, which is much higher than that of scandate cathode without film. Scandium (Sc) supplied by the film on the surface during the activation forms a Ba–Sc–O active layer, which helps to the emission.  相似文献   

18.
Developing a scalable approach to construct efficient and multifunctional electrodes for the hydrogen evolution reaction (HER), oxygen evolution reaction (OER), and oxygen reduction reaction (ORR) is an urgent need for overall water splitting and zinc–air batteries. In this work, a freestanding 3D heterostructure film is synthesized from a Ni-centered metal−organic framework (MOF)/graphene oxide. During the pyrolysis process, 1D carbon nanotubes formed from the MOF link with the 2D reduced graphene oxide sheets to stitch the 3D freestanding film. The results of the experiments and theoretical calculations show that the synergistic effect of the N-doped carbon shell and Ni nanoparticles leads to an optimized film with excellent electrocatalytic activity. Low overpotentials of 95 and 260 mV are merely needed for HER and OER, respectively, to reach a current density of 10 mA cm−2. In addition, a high half-wave potential of 0.875 V is obtained for the ORR, which is comparable to that of Pt/RuO2 and ranks among the top of non-noble-metal catalysts. The use of an “all-in-one” film as the electrode leads to excellent performance of the homemade water electrolyzer and zinc–air battery, indicating the potential of the film for practical applications.  相似文献   

19.
20.
Pb(Zr0.52Ti0.48)O3 thick films embedded with ZnO nanoneedles (PZT–ZnOn) were successfully prepared on Pt/Cr/SiO2/Si substrates by the hybrid sol–gel method via spin-coating ZnOn suspension and lead zirconate titanate (PZT) sol. To control the orientation of the films, a PbTiO3 (PT) layer was first deposited as a seed layer. Effects of annealing method and ZnOn contents on the corresponding orientation and crystallization of PZT–ZnOn films were investigated by XRD and SEM. The results show that all the PZT–ZnOn composite thick films have pure perovskite structure and high-quality film surface. The dielectric and ferroelectric properties of the PZT–ZnOn films are close to the PZT films, and have a little decrease with the increasing of the ZnOn contents.  相似文献   

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