Silicon anode solid-state batteries
Research on solid-state batteries has focused on lithium metal anodes. Alloy-based anodes have received less attention in part due to their lower specific capacity even though they should be safer. Tan
et al
. developed a slurry-based approach to create films from micrometer-scale silicon particles that can be used in anodes with carbon binders. When incorporated into solid-state batteries, they showed good performance across a range of temperatures and excellent cycle life in full cells. —MSL
Confining molecules in the nanoscale environment can lead to dramatic changes of their physical and chemical properties, which opens possibilities for new applications. There is a growing interest in liquefied gas electrolytes for electrochemical devices operating at low temperatures due to their low melting point. However, their high vapor pressure still poses potential safety concerns for practical usages. Herein, we report facile capillary condensation of gas electrolyte by strong confinement in sub-nanometer pores of metal-organic framework (MOF). By designing MOF-polymer membranes (MPMs) that present dense and continuous micropore (~0.8 nm) networks, we show significant uptake of hydrofluorocarbon molecules in MOF pores at pressure lower than the bulk counterpart. This unique property enables lithium/fluorinated graphite batteries with MPM-based electrolytes to deliver a significantly higher capacity than those with commercial separator membranes (~500 mAh g−1 vs. <0.03 mAh g−1) at −40 °C under reduced pressure of the electrolyte.
To meet growing energy demands, degradation mechanisms of energy storage devices must be better understood. As a non‐destructive tool, X‐ray Computed Tomography (CT) has been increasingly used by the battery community to perform in situ experiments that can investigate dynamic phenomena. However, few have used X‐ray CT to study representative battery systems over long cycle lifetimes (>100 cycles). Here, the in situ CT study of Zn–Ag batteries is reported and the effects of current collector parasitic gassing over long‐term storage and cycling are demonstrated. Performance representative in situ CT cells are designed that can achieve >250 cycles at a high areal capacity of 12.5 mAh cm−2. Combined with electrochemical experiments, the effects of current collector parasitic gassing are revealed with micro‐scale CT. The volume expansion and evolution of ZnO and Zn depletion are quantified with cycling and elevated temperature testing. The experimental insights are utilized to develop larger form‐factor (4 cm2) cells with electrochemically compatible current collectors. With this, over 500 cycles at a high capacity of 12.5 mAh cm−2 for a 4 cm2 form‐factor are demonstrated. This work demonstrates that in situ X‐ray CT used in long cycle‐lifetime studies can be applied to examine a multitude of battery chemistries to improve performances.
Lithium metal has been an attractive candidate as a next-generation anode material. Despite its popularity, stability issues of lithium in the liquid electrolyte and the formation of lithium whiskers have kept it from practical use. Three-dimensional (3D) current collectors have been proposed as an effective method to mitigate whisker growth. Although extensive research has been done, the effects of three key parameters of the 3D current collectors, namely, the surface area, the tortuosity factor, and the surface chemistry, on the performance of lithium metal batteries remain elusive. Herein, we quantitatively studied the role of these three parameters by synthesizing four types of porous copper networks with different sizes of well-structured microchannels. X-ray microscale computed tomography (micro-CT) allowed us to assess the surface area, the pore size, and the tortuosity factor of the porous copper materials. A metallic Zn coating was also applied to study the influence of surface chemistry on the performance of the 3D current collectors. The effects of these parameters on the performance were studied in detail through scanning electron microscopy (SEM) and titration gas chromatography (TGC). Stochastic simulations further allowed us to interpret the role of the tortuosity factor in lithiation. The optimal range of the key parameters is thereby found for the porous coppers and their performance is predicted. Using these parameters to inform the design of porous copper anodes for Li deposition, Coulombic efficiencies (CEs) of up to 99.63% are achieved, thus paving the way for the design of effective 3D current collector systems.
A trap‐corrected bias–temperature–stress (TraC‐BTS) method to quantify the kinetics of ion migration in dielectrics based on capacitance–voltage measurements is presented. The method is based on the extraction of flatband potential (Vfb) shifts in metal–insulator–semiconductor test structures an enables the reliability assessment of semiconductor dielectrics and solar cells. Herein, it is shown that carrier trapping in the dielectric must be accounted for, as it strongly affects the measurement of flatband potential in silicon‐nitride‐based capacitors. This effect is corrected by isolating the contribution of trapping on Vfb using contamination‐free control devices. A specific drift‐diffusion model of the ion kinetics presented herein allows the extraction of ion diffusivity. An Arrhenius relationship is obtained for sodium diffusivity in silicon nitride in a temperature range from 30 °C to 90 °C at an electric field of 1 MV cm−1, yielding a prefactor and an activation energy , with a 95% confidence interval of [] eV for the diffusivity. These quantitative kinetics confirm that silicon nitride may be a poor sodium migration barrier under a significant electric field.
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