Characterization and Comparative Study of Energy Efficient Mechanochemically Induced NASICON Sodium Solid Electrolyte Synthesis.

In recent years, there is growing interest in solid-state electrolytes due to their many promising properties, making them key to the future of battery technology. This future depends among other things on easy processing technologies for the solid electrolyte. The sodium superionic conductor (NASICON) Na3 Zr2 Si2 PO12 is a promising sodium solid electrolyte; however, reported methods of synthesis are time consuming. To this effect, attempt was made to develop a simple time efficient alternative processing route. Firstly, a comparative study between a new method and commonly reported methods was carried out to gain a clear insight into the mechanism of formation of sodium superionic conductors (NASICON). It was observed that through a careful selection of precursors, and the use of high-energy milling (HEM) the NASICON conversion process was enhanced and optimized, this reduces the processing time and required energy, opening up a new alternative route for synthesis. The obtained solid electrolyte was stable during Na cycling vs. Na-metal at 1 mA cm-1 , and a room temperature conductivity of 1.8 mS cm-1 was attained.

Lithium Manganese Sulfates as a New Class of Supercapattery Materials at Elevated Temperatures.

To make supercapattery devices feasible, there is an urgent need to find electrode materials that exhibit a hybrid mechanism of energy storage. Herein, we provide a first report on the capability of lithium manganese sulfates to be used as supercapattery materials at elevated temperatures. Two compositions are studied: monoclinic Li2Mn(SO4)2 and orthorhombic Li2Mn2(SO4)3, which are prepared by a freeze-drying method followed by heat treatment at 500 °C. The electrochemical performance of sulfate electrodes is evaluated in lithium-ion cells using two types of electrolytes: conventional carbonate-based electrolytes and ionic liquid IL ones. The electrochemical measurements are carried out in the temperature range of 20-60 °C. The stability of sulfate electrodes after cycling is monitored by in-situ Raman spectroscopy and ex-situ XRD and TEM analysis. It is found that sulfate salts store Li+ by a hybrid mechanism that depends on the kind of electrolyte used and the recording temperature. Li2Mn(SO4)2 outperforms Li2Mn2(SO4)3 and displays excellent electrochemical properties at elevated temperatures: at 60 °C, the energy density reaches 280 Wh/kg at a power density of 11,000 W/kg. During cell cycling, there is a transformation of the Li-rich salt, Li2Mn(SO4)2, into a defective Li-poor one, Li2Mn2(SO4)3, which appears to be responsible for the improved storage properties. The data reveals that Li2Mn(SO4)2 is a prospective candidate for supercapacitor electrode materials at elevated temperatures.

Eu- and Tb-adsorbed Si3N4 and Ge3N4: tuning the colours with one luminescent host.

Phosphor-converted white light emitting diodes (pc-LEDs) are efficient light sources for applications in lighting and electronic devices. Nitrides, with their wide-ranging applicability due to their intriguing structural diversity, and their auspicious chemical and physical properties, represent an essential component in industrial and materials applications. Here, we present the successful adsorption of Eu and Tb at the grain boundaries of bulk ß-Si3N4 and ß-Ge3N4 by a successful combustion synthesis. The adsorption of europium and terbium, and the synergic combination of both, resulted in intriguing luminescence properties of all compounds (red, green, orange and yellow). In particular, the fact that one host can deliver different colours renders Eu,Tb-ß-M3N4 (M = Si, Ge) a prospective chief component for future light emitting diodes (LEDs). For the elucidation of the electronic properties and structure of ß-Si3N4 and ß-Ge3N4, Mott-Schottky (MS) measurements and density functional theory (DFT) computations were conducted for the bare and RE adsorbed samples.

Data-driven capacity estimation of commercial lithium-ion batteries from voltage relaxation.

Accurate capacity estimation is crucial for the reliable and safe operation of lithium-ion batteries. In particular, exploiting the relaxation voltage curve features could enable battery capacity estimation without additional cycling information. Here, we report the study of three datasets comprising 130 commercial lithium-ion cells cycled under various conditions to evaluate the capacity estimation approach. One dataset is collected for model building from batteries with LiNi0.86Co0.11Al0.03O2-based positive electrodes. The other two datasets, used for validation, are obtained from batteries with LiNi0.83Co0.11Mn0.07O2-based positive electrodes and batteries with the blend of Li(NiCoMn)O2 - Li(NiCoAl)O2 positive electrodes. Base models that use machine learning methods are employed to estimate the battery capacity using features derived from the relaxation voltage profiles. The best model achieves a root-mean-square error of 1.1% for the dataset used for the model building. A transfer learning model is then developed by adding a featured linear transformation to the base model. This extended model achieves a root-mean-square error of less than 1.7% on the datasets used for the model validation, indicating the successful applicability of the capacity estimation approach utilizing cell voltage relaxation.

Closing the yellow gap with Eu- and Tb-doped GaN: one luminescent host resulting in three colours.

Gallium nitride (GaN) is a key material when it comes to light-emitting diodes (LEDs) and has pushed the LED revolution in lighting and displays. The concept of down-conversion of a GaN-based blue LED offers the possibility to provide efficient generation of monochromatic, high-color purity light resulting in a highly efficient warm-white all-nitride phosphor-converted light emitting diode (pc-LED). Although the down conversion of blue light from InGaN LEDs has become a dominant technique for producing white light, there are still some technical challenges, e.g. the immiscibility of GaN and InN and the lattice mismatch between the substrate and InGaN, that have to be overcome. Here we demonstrate the doping of bulk GaN with europium, terbium and the combination of both resulting in intriguing luminescence properties, pushing the role of GaN:Eu,Tb as a chief component in future light emitting diodes. This colour tuning proves that one luminescence host can provide three colours (red, green and orange) and that even the so called "yellow gap" could be closed with a III-nitride. By using one material for all colours, it will be possible to overcome the technical challenges in building up LED devices, which will open up new capabilities for modern highly efficient phosphors.

Synthesis and Characterization of a Multication Doped Mn Spinel, LiNi0.3Cu0.1Fe0.2Mn1.4O4, as 5 V Positive Electrode Material.

The suitability of multication doping to stabilize the disordered Fd3̅m structure in a spinel is reported here. In this work, LiNi0.3Cu0.1Fe0.2Mn1.4O4 was synthesized via a sol-gel route at a calcination temperature of 850 °C. LiNi0.3Cu0.1Fe0.2Mn1.4O4 is evaluated as positive electrode material in a voltage range between 3.5 and 5.3 V (vs Li+/Li) with an initial specific discharge capacity of 126 mAh g-1 at a rate of C/2. This material shows good cycling stability with a capacity retention of 89% after 200 cycles and an excellent rate capability with the discharge capacity reaching 78 mAh g-1 at a rate of 20C. In operando X-ray diffraction (XRD) measurements with a laboratory X-ray source between 3.5 and 5.3 V at a rate of C/10 reveal that the (de)lithiation occurs via a solid-solution mechanism where a local variation of lithium content is observed. A simplified estimation based on the in operando XRD analysis suggests that around 17-31 mAh g-1 of discharge capacity in the first cycle is used for a reductive parasitic reaction, hindering a full lithiation of the positive electrode at the end of the first discharge.