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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.

This paper is a collection of selected contributions of the 1st International Workshop on Mechanochemistry of Metal Hydrides that was held in Oslo in May 2018. In this paper, the recent developments in the use of mechanochemistry to synthesize and modify metal hydrides are reviewed. A special emphasis is made on new techniques beside the traditional way of ball milling. High energy milling, ball milling under hydrogen reactive gas, cryomilling and severe plastic deformation techniques such as High-Pressure Torsion (HPT), Surface Mechanical Attrition Treatment (SMAT) and cold rolling are discussed. The new characterization method of in-situ X-ray diffraction during milling is described.

Rechargeable solid-state magnesium batteries are considered for high energy density storage and usage in mobile applications as well as to store energy from intermittent energy sources, triggering intense research for suitable electrode and electrolyte materials. Recently, magnesium borohydride, Mg(BH 4) 2 , was found to be an effective precursor for solid-state Mg-ion conductors. During the mechanochemical synthesis of these Mg-ion conductors, amorphous Mg(BH 4) 2 is typically formed and it was postulated that this amorphous phase promotes the conductivity. Here, electrochemical impedance spectroscopy of as-received γ-Mg(BH 4) 2 and ball milled, amorphous Mg(BH 4) 2 confirmed that the conductivity of the latter is ~2 orders of magnitude higher than in as-received γ-Mg(BH 4) 2 at 353 K. Pair distribution function (PDF) analysis of the local structure shows striking similarities up to a length scale of 5.1 Å, suggesting similar conduction pathways in both the crystalline and amorphous sample. Up to 12.27 Å the PDF indicates that a 3D net of interpenetrating channels might still be present in the amorphous phase although less ordered compared to the as-received γ-phase. However, quasi elastic neutron scattering experiments (QenS) were used to study the rotational mobility of the [BH 4 ] units, revealing a much larger fraction of activated [BH 4 ] rotations in amorphous Mg(BH 4) 2. These findings suggest that the conduction process in amorphous Mg(BH 4) 2 is supported by stronger rotational mobility, which is proposed to be the so-called "paddle-wheel" mechanism. Energy storage is one of the grand challenges for present and future generations. In recent years, intermittent renewable energy production has increased worldwide resulting in a high demand for energy storage systems. "Beyond Li-batteries", which are all-solid-state batteries with alternative working ions, including Na and Mg, are considered a promising alternative as they are cheaper and with respect to their natural abundancy more sustainable. However, the transport properties of larger Na + or double-charged Mg 2+ are challenging and directly correlated to the underlying crystal structure and dynamics. Understanding the accompanying structural and dynamic changes as well as finding high-performance cathode materials remain bottlenecks for the improvement of Mg-ion batteries 1. Mg-ion batteries (MIBs) have several advantages compared to Li-ion technology 2. For instance, the low electrochemical potential of −2.4 V (vs. standard hydrogen electrode (SHE)) is close to the one of Li with −3.0 V of Li/Li + , which allows for high cell voltages. Furthermore, Mg metal has a higher volumetric capacity of 3833 mA•cm −3 compared to 2036 mAh•cm −3 of Li metal, and magnesium has a higher natural abundancy of

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In this work, praseodymium(iii) borohydride, Pr(BH4)3, and an isotopically enriched analogue, Pr(11BD4)3, are prepared by a new route via a solvate complex, Pr(11BD4)3S(CH3)2. Nd(BH4)3 was synthesized using the same method and the structures, polymorphic transformations, and thermal stabilities of these compounds are investigated in detail. α-Pr(BH4)3 and α-Nd(BH4)3 are isostructural with cubic unit cells (Pa3[combining macron]) stable at room temperature (RT) and a unit cell volume per formula unit (V/Z) of 180.1 and 175.8 Å3, respectively. Heating α-Pr(BH4)3 to T ∼ 190 °C, p(Ar) = 1 bar, introduces a transition to a rhombohedral polymorph, r-Pr(BH4)3 (R3[combining macron]c) with a smaller unit cell volume and a denser structure, V/Z = 156.06 Å3. A similar transition was not observed for Nd(BH4)3. However, heat treatment of α-Pr(BH4)3, at T ∼ 190 °C, p(H2) = 40 bar and α-Nd(BH4)3, at T ∼ 270 °C, p(H2) = 98 bar facilitates reversible formation of another three cubic polymorph, denoted as β, β' and β''-RE(BH4)3 (Fm3[combining macron]c). Moreover, the transition β- to β'- to β''- is considered a rare example of stepwise negative thermal expansion. For Pr(BH4)3, ∼2/3 of the sample takes this route of transformation whereas in argon only ∼5 wt%, and the remaining transforms directly from α- to r-Pr(BH4)3. The β-polymorphs are porous with V/Z = 172.4 and 172.7 Å3 for β''-RE(BH4)3, RE = Pr or Nd, respectively, and are stabilized by the elevated hydrogen pressures. The polymorphic transitions occur due to rotation of RE(BH4)6 octahedra without breaking or forming chemical bonds. Structural DFT optimization reveals the decreasing stability of α-Pr(BH4)3 > β-Pr(BH4)3 > r-Pr(BH4)3.

Hydrogen as an energy carrier is very versatile in energy storage applications. Developments in novel, sustainable technologies towards a CO2-free society are needed and the exploration of all-solid-state batteries (ASSBs) as well as solid-state hydrogen storage applications based on metal hydrides can provide solutions for such technologies. However, there are still many technical challenges for both hydrogen storage material and ASSBs related to designing low-cost materials with low-environmental impact. The current materials considered for all-solid-state batteries should have high conductivities for Na+, Mg2+ and Ca2+, while Al3+-based compounds are often marginalised due to the lack of suitable electrode and electrolyte materials. In hydrogen storage materials, the sluggish kinetic behaviour of solid-state hydride materials is one of the key constraints that limit their practical uses. Therefore, it is necessary to overcome the kinetic issues of hydride materials before discussing and considering them on the system level. This review summarizes the achievements of the Marie Skłodowska-Curie Actions (MSCA) innovative training network (ITN) ECOSTORE, the aim of which was the investigation of different aspects of (complex) metal hydride materials. Advances in battery and hydrogen storage materials for the efficient and compact storage of renewable energy production are discussed.