In recent years, the concept of entropy stabilization of crystal structures in oxide systems has led to an increased research activity in the field of “high entropy oxides”. These compounds comprise the incorporation of multiple metal cations into single-phase crystal structures and interactions among the various metal cations leading to interesting novel and unexpected properties. Here, we report on the reversible lithium storage properties of the high entropy oxides, the underlying mechanisms governing these properties, and the influence of entropy stabilization on the electrochemical behavior. It is found that the stabilization effect of entropy brings significant benefits for the storage capacity retention of high entropy oxides and greatly improves the cycling stability. Additionally, it is observed that the electrochemical behavior of the high entropy oxides depends on each of the metal cations present, thus providing the opportunity to tailor the electrochemical properties by simply changing the elemental composition.

Multicomponent rare earth oxide (REO) nanocrystalline powders containing up to seven equiatomic rare earth elements were successfully synthesized in a single-phase CaF₂-type (Fm-3 m) structure. The addition of more than six elements resulted in the formation of a secondary phase. Annealing at 1000°C for 1 h led to the formation of a single-phase (Ia-3) even in the 7-component system. In the absence of cerium (Ce⁴⁺), secondary phases were observed irrespective of the number of cations or the extent of thermal treatment indicating that cerium cations played a crucial role in stabilizing the multicomponent REOs into a phase pure structure. GRAPHICAL ABSTRACT IMPACT STATEMENT Multicomponent equiatomic rare earth oxides pioneer a new group of materials that crystallize into a single-phase structure with the dominant role of a single element instead of entropy.

Here we report for the first time the development of a Mg rechargeable battery using a graphene–sulfur nanocomposite as the cathode, a Mg–carbon composite as the anode and a non-nucleophilic Mg based complex in tetraglyme solvent as the electrolyte. The graphene–sulfur nanocomposites are prepared through a new pathway by the combination of thermal and chemical precipitation methods. The Mg/S cell delivers a higher reversible capacity (448 mA h g⁻¹), a longer cyclability (236 mA h g⁻¹ at the end of the 50^th cycle) and a better rate capability than previously described cells. The dissolution of Mg polysulfides to the anode side was studied by X-ray photoelectron spectroscopy. The use of a graphene–sulfur composite cathode electrode, with the properties of a high surface area, a porous morphology, a very good electronic conductivity and the presence of oxygen functional groups, along with a non-nucleophilic Mg electrolyte gives an improved battery performance.

High entropy oxides (HEOs) with chemically disordered multi-cation structure attract intensive interest as negative electrode materials for battery applications. The outstanding electrochemical performance has been attributed to the high-entropy stabilization and the so-called ‘cocktail effect’. However, the configurational entropy of the HEO, which is thermodynamically only metastable at room-temperature, is insufficient to drive the structural reversibility during conversion-type battery reaction, and the ‘cocktail effect’ has not been explained thus far. This work unveils the multi-cations synergy of the HEO Mg_0.2Co_0.2Ni_0.2Cu_0.2Zn_0.2O at atomic and nanoscale during electrochemical reaction and explains the ‘cocktail effect’. The more electronegative elements form an electrochemically inert 3-dimensional metallic nano-network enabling electron transport. The electrochemical inactive cation stabilizes an oxide nanophase, which is semi-coherent with the metallic phase and accommodates Li⁺ ions. This self-assembled nanostructure enables stable cycling of micron-sized particles, which bypasses the need for nanoscale pre-modification required for conventional metal oxides in battery applications. This demonstrates elemental diversity is the key for optimizing multi-cation electrode materials.