Seyedabolfazl Mousavihashemi

Ni‐rich layered oxides, such as LiNi _0.8 Mn _0.1 Co _0.1 O ₂ (NMC811), offer high capacity but suffer from structural degradation and rapid fading under extended cycling. Herein, Mg doping as a structural stabilization strategy, directly comparing incorporation via precursor coprecipitation, solid‐state lithiation, and a novel two‐step route is introduced. All Mg doped NMC811 compositions show reduced cation mixing and enhanced cycling stability, with 0.1% Mg yielding the most favorable lattice evolution as revealed by operando X‐ray diffraction. For the first time, operando electrochemical dilatometry is utilized to investigate the doped NMC811, revealing direct correlations between electrode volume changes and electrochemical behaviour. While Mg primarily suppresses structural degradation, the solid‐state lithiation route delivers the greatest performance gains, outperforming both coprecipitation and the combined approach. This work demonstrates that targeted Mg incorporation can noticeably extend the lifetime of Ni‐rich cathodes and establishes operando dilatometry as a powerful tool for linking atomic‐scale stabilization strategies with macroscopic electrode mechanics.

Modern batteries are highly complex devices. The cells contain many components—which in turn all have many variations, both in terms of chemistry and physical properties. A few examples: the active materials making the electrodes are coated on current collectors using solvents, binders and additives; the multicomponent electrolyte, contains salts, solvents, and additives; the electrolyte can also be a solid ceramic, polymer or a glass material; batteries also contain a separator, which can be made of glass fibres, polymeric, ceramic, composite, etc. Moving up in scale all these components are assembled in cells of different formats and geometries, coin cells and Swagelok cells for funamental testing and understanding, and pouch, prismatic and cylindrical cells for application. Given this complexity dictated by so many components and variations, there is no wonder that addressing the crucial issue of true sustainability is an extremely challenging task. How can we make sure that each component is sustainable? How can the performance can be delivered using more sustainable battery components? What actions do we need to take to address battery sustainability properly? How do we actually qualify and quantify the sustainability in the best way possible? And perhaps most importantly; how can we all work—academia and battery industry together—to enable the latter to manufacture more sustainable batteries for a truly cleaner future? This Roadmap assembles views from experts from academia, industry, research institutes, and other organisations on how we could and should achieve a more sustainable battery future. The palette has many colours: it discusses the very definition of a sustainable battery, the need for diversification beyond lithium-ion batteries (LIBs), the importance of sustainability assessments, the threat of scarcity of raw materials and the possible impact on future manufacturing of LIBs, the possibility of more sustainable cells by electrode and electrolyte chemistries as well as manufacturing, the important role of new battery chemistries, the crucial role of AI and automation in the discovery of the truly sustainable batteries of the future and the importance of developimg a circular battery economy.

The widespread use of high‐capacity Ni‐rich layered oxides such as LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811), in lithium‐ion batteries is hindered due to practical capacity loss and reduced working voltage during operation. Aging leads to defective NMC811 particles, affecting electrochemical performance. Surface modification offers a promising approach to improve cycle life. Here, we introduce an amorphous lithium titanate (LTO) coating via atomic layer deposition (ALD), not only covering NMC811 surfaces but also penetrating cavities and grain boundaries. As NMC811 electrodes suffer from low structural stability during charge and discharge, We combined electrochemistry, operando X‐ray diffraction (XRD), and dilatometry to understand structural changes and the coating protective effects. XRD reveals significant structural evolution during delithiation for uncoated NMC811. The highly reversible phase change in coated NMC811 highlights enhanced bulk structure stability. The LTO coating retards NMC811 degradation, boosting capacity retention from 86 % to 93 % after 140 cycles. This study underscores the importance of grain boundary engineering for Ni‐rich layered oxide electrode stability and the interplay of chemical and mechanical factors in battery aging.

In this study, the performance of a binder‐free LiNi _0.6 Co _0.2 Mn _0.2 O ₂ (NMC622) positive electrode utilizing single‐walled carbon nanotubes (SWCNTs) is investigated and compared to the conventional state‐of‐the‐art NMC622 composite positive electrode. The binder‐free electrode has been prepared without using toxic and expensive N ‐Methyl‐2‐pyrrolidone (NMP) solvent and it is free‐standing that allows a wider range of applications such as flexible devices. Electrochemical techniques such as cyclic voltammetry, electrochemical impedance spectroscopy, and galvanostatic charge–discharge reveal that the binder‐free positive electrode performance is similar to the conventional composite cathodes, deducing that only ≈1% of SWCNTs perform well not only as a conductive agent but also as a binder. The NMC622 composite electrode with SWCNTs provided specific capacity of 135.8 mAh g ⁻¹ at a 5C rate during discharge, with above 97% capacity retention after the rate capability test in a half cell.

Supervalent doping is one of the most common methods used to stabilize the highly conductive cubic phase of Li₇La₃Zr₂O₁₂ (LLZO) solid electrolytes. While several different doping elements have shown that they are capable of stabilizing the cubic LLZO structure, there is still no clear consensus as to an optimal doping strategy. In this study we present one of the most extensive comparative analyses on supervalent doping of LLZO done to date. Herein, we compare the effects of eight different doping elements (Al, Ga, Fe, Ta, Nb, Sb, W and Mo) on the synthesis, crystal structure, morphology, and electrochemical properties of LLZO. We also propose a new guideline that would allow for the quick and easy identification of doping elements in LLZO and the estimation of their concentration using Raman spectroscopy. Our results show how Ga doping leads to exceptionally high ionic conductivities (1.30 × 10⁻³ S cm⁻¹) and low activation energies (0.26 eV) due to changes in the crystal symmetry of LLZO. On top of that, Ga doping also significantly lowers the required synthesis temperatures and increases the relative density of the LLZO structure, making Ga the most suitable element for LLZO doping. On the other hand, Nb doping shows the lowest ionic conductivity (1.91 × 10⁻⁴ S cm⁻¹) and a high activation energy (0.44 eV) of the investigated dopants, due to a poor sintering performance.