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.

High‐entropy materials, especially high‐entropy alloys and oxides, have gained significant interest over the years due to their unique structural characteristics and correlated possibilities for tailoring of functional properties. The developments in the area of high‐entropy oxides are highlighted here, with emphasis placed on their fundamental understanding, including entropy‐dominated phase‐stabilization effects and prospective applications, e.g., in the field of electrochemical energy storage. Critical comments on the different classes of high‐entropy oxides are made and the underlying principles for the observed properties are summarized. The diversity of materials design, provided by the entropy‐mediated phase‐stabilization concept, allows engineering of new oxide candidates for practical applications, warranting further studies in this emerging field of materials science.

An overview of high-entropy materials for energy applications, including H₂ catalysis and storage, CO₂ conversion, O₂ catalysis and electrochemical energy storage, is given and the challenges and opportunities within this field are discussed.

Charge and discharge of lithium ion battery electrodes is accompanied by severe volume changes. In a confined space, the volume cannot expand, leading to significant pressures induced by local microstructural changes within the battery. While volume changes appear to be less critical in batteries with liquid electrolytes, they will be more critical in the case of lithium ion batteries with solid electrolytes and they will be even more critical and detrimental in the case of all-solid-state batteries with a lithium metal electrode. In this work we first summarize, compare, and analyze the volume changes occurring in state of the art electrode materials, based on crystallographic studies. A quantitative analysis follows that is based on the evaluation of the partial molar volume of lithium as a function of the degree of lithiation for different electrode materials. Second, the reaction volumes of operating full cells (“charge/discharge volumes”) are experimentally determined from pressure-dependent open-circuit voltage measurements. The resulting changes in the open-circuit voltage are in the order of 1 mV/100 MPa, are well measurable, and agree with changes observed in the crystallographic data. Third, the pressure changes within solid-state batteries are approximated under the assumption of incompressibility, i.e. for constant volume of the cell casing, and are compared to experimental data obtained from model-type full cells. In addition to the understanding of the occurring volume changes of electrode materials and resulting pressure changes in solid-state batteries, we propose “mechanical” blending of electrode materials to achieve better cycling performance when aiming at “zero-strain” electrodes.