As the most promising anode material for sodium-ion batteries (SIBs), elemental phosphorus (P) has recently gained a lot of interest due to its extraordinary theoretical capacity of 2596 mAh/g. The main drawback of a P anode is its low conductivity and rapid structural degradation caused by the enormous volume expansion (>490%) during cycling. Here, we redesigned the anode structure by using an innovative methodology to fabricate flexible paper made of nitrogen-doped graphene and amorphous phosphorus that effectively tackles this problem. The restructured anode exhibits an ultrastable cyclic performance and excellent rate capability (809 mAh/g at 1500 mA/g). The excellent structural integrity of the novel anode was further visualized during cycling by using in situ experiments inside a high-resolution transmission electron microscope (HRTEM), and the associated sodiation/desodiation mechanism was also thoroughly investigated. Finally, density functional theory (DFT) calculations confirmed that the N-doped graphene not only contributes to an increase in capacity for sodium storage but also is beneficial in regards to improved rate performance of the anode.
The development of rechargeable batteries with high performance is considered to be a feasible way to satisfy the increasing needs of electric vehicles and portable devices. It is of vital importance to design electrodes with high electrochemical performance and to understand the nature of the electrode/electrolyte interfaces during battery operation, which allows a direct observation of the complicated chemical and physical processes within the electrodes and electrolyte, and thus provides real-time information for further design and optimization of the battery performance. Here, the recent progress in in situ techniques employed for the investigations of material structural evolutions is described, including characterization using neutrons, X-ray diffraction, and nuclear magnetic resonance. In situ techniques utilized for in-depth uncovering the electrode/electrolyte phase/interface change mechanisms are then highlighted, including transmission electron microscopy, atomic force microscopy, X-ray spectroscopy, and Raman spectroscopy. The real-time monitoring of lithium dendrite growth and in situ detection of gas evolution during charge/discharge processes are also discussed. Finally, the major challenges and opportunities of in situ characterization techniques are outlined toward new developments of rechargeable batteries, including innovation in the design of compatible in situ cells, applications of dynamic analysis, and in situ electrochemistry under multi-stimuli. A clear and in-depth understanding of in situ technique applications and the mechanisms of structural evolutions, surface/interface changes, and gas generations within rechargeable batteries is given here.
Although extensive studies have been done on lead-free dielectric ceramics to achieve excellent dielectric behaviors and good energy storage performance, the major problem of low energy density has not been solved so far. Here, we report on designing the crossover relaxor ferroelectrics (CRFE), a crossover region between the normal ferroelectrics and relaxor ferroelectrics, as a solution to overcome the low energy density. CRFE exhibits smaller free energy and lower defect density in the modified Landau theory, which helps to obtain ultrahigh energy density and efficiency. The (1–x)Ba0.65Sr0.35TiO3–xBi(Mg2/3Nb1/3)O3 ((1–x)BST–xBMN) (x = 0, 0.08, 0.1, 0.18, 0.2) ceramic was synthesized by a solid-state reaction method. The solid solutions exhibit dielectric frequency dispersion, which suggests typical relaxor characteristics with the increasing BMN content. The crossover ferroelectrics of 0.9BST–0.1BMN ceramic possesses a high energy storage efficiency (η) of 85.71%, a high energy storage density (W) of 3.90 J/cm3, and an ultrahigh recoverable energy storage density (W rec) of 3.34 J/cm3 under a dielectric breakdown strength of 400 kV/cm and is superior to other lead-free BaTiO3 (BT)-based energy storage ceramics. It also exhibits strong thermal stability in the temperature range from 25 to 150 °C under an electric field of 300 kV/cm, with the fluctuations below 3% and with the energy storage density and energy efficiency at about 2.8 J/cm3 and 82.93%, respectively. The enhanced recoverable energy density and breakdown strength of BT-based materials with significantly high energy efficiency make it a promising candidate to meet the wide requirements for high power applications.
Heating mechanisms and particle flow balancing of capacitively coupled plasmas driven by combined dc/rf sources have been investigated by particle-in-cell/Monte Carlo simulations. At low pressure, Ohmic heating will be suppressed and stochastic heating will be enhanced while increasing dc voltage. But the overall heating power will decrease. No heating mode transitions are observed. At high pressure, bulk plasma density decreases at low dc and rf voltage, and the one-side α-γ transition will occur while increasing dc voltage. After the transition, the plasma density abruptly increases and average electron energy drops. As the result of that, the plasma is sustained by secondary electrons instead of the Ohmic heating of the bulk electrons. The dc source will reduce, or even eliminate at high voltage, the electron charge flowing into the dc powered electrode. Therefore the ratio of electron-to-ion charge flowing into the rf powered electrode over one period increases from −1.0 to −2.0–−2.3 for low pressure and −2.2–−5.0 for high pressure.
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