Three types of next generation batteries are currently being envisaged among the international community: metal-air batteries, multivalent cation batteries and all-solid-state batteries. These battery designs require high-performance, safe and cost effective electrolytes that are compatible with optimized electrode materials. Solid electrolytes have not yet been extensively employed in commercial batteries as they suffer from poor ionic conduction at acceptable temperatures and insufficient stability with respect to lithium-metal. Here we show a novel type of glasses, which evolve from an antiperovskite structure and that show the highest ionic conductivity ever reported for the Li-ion (25 mS cm À1 at 25 C). These glassy electrolytes for lithium batteries are inexpensive, light, recyclable, non-flammable and non-toxic.Moreover, they present a wide electrochemical window (higher than 8 V) and thermal stability within the application range of temperatures.
The advent of a Li+ or Na+ glass electrolyte with a cation conductivity σi > 10−2 S cm−1 at 25 °C and a motional enthalpy ΔHm = 0.06 eV that is wet by a metallic lithium or sodium anode is used to develop a new strategy for an all-solid-state, rechargeable, metal-plating battery.
Precursors of the crystalline antiperovskites A3−xHxOCl (A = Li or Na and 0 < x < 1) can be rendered glass/amorphous solid Li+ or Na+ electrolytes by the addition of water to its solvation limit with/without the addition of a small amount of an oxide or hydroxide.
A thermodynamic assessment of the Bi-Sn-Zn ternary system was carried out using the CALPHAD approach along with thermodynamic descriptions from new assessments of the Bi-Sn and Bi-Zn systems. Selected experimental data from the literature and our own work were also used. New sets of optimized thermodynamic parameters were obtained that lead to a very good fit between the calculated and experimental data. The Bi-Sn-Zn system is one of the candidates for lead-free solder materials.
A room-temperature all-solid-state rechargeable battery cell containing a tandem electrolyte consisting of a Li-glass electrolyte in contact with a lithium anode and a plasticizer in contact with a conventional, low cost oxide host cathode was charged to 5 V versus lithium with a charge/discharge cycle life of over 23,000 cycles at a rate of 153 mA·g of active material. A larger positive electrode cell with 329 cycles had a capacity of 585 mAh·g at a cutoff of 2.5 V and a current of 23 mA·g of the active material; the capacity rose with cycle number over the 329 cycles tested during 13 consecutive months. Another cell had a discharge voltage from 4.5 to 3.7 V over 316 cycles at a rate of 46 mA·g of active material. Both the Li-glass electrolyte and the plasticizer contain electric dipoles that respond to the internal electric fields generated during charge by a redistribution of mobile cations in the glass and by extraction of Li from the active cathode host particles. The electric dipoles remain oriented during discharge to retain an internal electric field after a discharge. The plasticizer accommodates to the volume changes in the active cathode particles during charge/discharge cycling and retains during charge the Li extracted from the cathode particles at the plasticizer/cathode-particle interface; return of these Li to the active cathode particles during discharge only involves a displacement back across the plasticizer/cathode interface and transport within the cathode particle. A slow motion at room temperature of the electric dipoles in the Li-glass electrolyte increases with time the electric field across the EDLC of the anode/Li-glass interface to where Li from the glass electrolyte is plated on the anode without being replenished from the cathode, which charges the Li-glass electrolyte negative and consequently the glass side of the Li-glass/plasticizer EDLC. Stripping back the Li to the Li-glass during discharge is enhanced by the negative charge in the Li-glass. Since the Li-glass is not reduced on contact with metallic lithium, no passivating interface layer contributes to a capacity fade; instead, the discharge capacity increases with cycle number as a result of dipole polarization in the Li-glass electrolyte leading to a capacity increase of the Li-glass/plasticizer EDLC. The storage of electric power by both faradaic electrochemical extraction/insertion of Li in the cathode and electrostatic stored energy in the EDLCs provides a safe and fast charge and discharge with a long cycle life and a greater capacity than can be provided by the cathode host extraction/insertion reaction. The cell can be charged to a high voltage versus a lithium anode because of the added charge of the EDLCs.
The binary Bi-Sn was studied by means of SEM (Scanning Electron Microscopy)/EDS (Energy-Dispersive solid state Spectrometry), DTA (Differential Thermal Analysis)/DSC (Differential Scanning Calorimetry) and RT-XRD (Room Temperature X-Ray Diffraction) in order to clarify discrepancies concerning the Bi reported solubility in (Sn). It was found that (Sn) dissolves approximately 10 wt% of Bi at the eutectic temperature.The experimental effort for the Bi-Zn system was limited to the investigation of the discrepancies concerning the solubility limit of Zn in (Bi) and the solubility of Bi in (Zn). Results indicate that the solubility of both elements in the respective solid solution is approximately 0.3 wt% at 200 • C.Three different features were studied within the Bi-Sn-Zn system. Although there are enough data to establish the liquid miscibility gap occurring in the phase diagram of binary Bi-Zn, no data could be found for the ternary. Samples belonging to the isopleths with w(Bi) ∼ 10% and w(Sn) ∼ 5%, 13% and 19% were measured by DTA/DSC. The aim was to characterize the miscibility gap in the liquid phase. Samples belonging to the isopleths with w(Sn) ∼ 40%, 58%, 77/81% and w(Zn) ∼ 12% were also measured by DTA/DSC to complement the study of Bi-Sn-Zn. Solubilities in the solid terminal solutions were determined by SEM/EDS. Samples were also analyzed by RT-XRD and HT-XRD (High Temperature X-Ray Diffraction) confirming the DTA/DSC results for solid state phase equilibria.
Electrostatic gating of two-dimensional (2D) materials with ionic liquids (ILs), leading to the accumulation of high surface charge carrier densities, has been often exploited in 2D devices. However, the intrinsic liquid nature of ILs, their sensitivity to humidity, and the stress induced in frozen liquids inhibit ILs from constituting an ideal platform for electrostatic gating. Here we report a lithium-ion solid electrolyte substrate, demonstrating its application in highperformance back-gated n-type MoS 2 and p-type WSe 2 transistors with sub-threshold values approaching the ideal limit of 60 mV/dec and complementary inverter amplifier gain of 34, the highest among comparable amplifiers. Remarkably, these outstanding values were obtained under 1 V power supply. Microscopic studies of the transistor channel using microwave impedance microscopy reveal a homogeneous channel formation, indicative of a smooth interface between the TMD and underlying electrolytic substrate. These results establish lithium-ion substrates as a promising alternative to ILs for advanced thin-film devices.
The ability for electrochemical cells to self-charge for extended periods of time is desirable for energy storage applications. While self-oscillation is a phenomenon found in human-made dynamic systems and in nature, its appearance in electrochemical cells has not been reported or anticipated. Here, we chose an electrochemical cell containing two electrodes separated by a self-organizing glass electrolyte containing alkali cations. The ferroelectric character of the electrolyte, with an impressively high dielectric constant of 106–107, supported self-charge and self-oscillation. After fabrication, the cells were characterized to determine the electrical impedance, dielectric spectroscopy, and electrochemical discharge. The electrochemical cells also displayed negative resistance and negative capacitance. Negative capacitance is due to the formation of an inverted capacitor between the double-layer capacitor formed at the negative electrode/electrolyte interface and the dipoles of the ferroelectric-electrolyte. Negative resistance is triggered by the formation of an interface phase, which leads to a step-change of the chemical potential of the electrode. The electrochemical cell demonstrates an entanglement between negative resistance, negative capacitance, self-charge, self-cycling, and the activation energy vs thermal energy or external work. The phenomenon of self-cycling is enhanced at low temperatures where the activation energy is higher than the thermal energy. This demonstration extends the Landau-Khalatnikov model for a ferroelectric to a bistable device in which the bistability resides in an electrode. The results reported here reveal the first report of negative capacitance and negative resistance existing in the same process, which can lead to valuable advancements in energy storage devices and in low-frequency applications.
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