Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries

Abstract

Cation-disordered rocksalt-type high-entropy cathodes for Li-ion batteries.

High-entropy ceramics: Present status, challenges, and a look forward

“…Solid state reaction synthesis is the most commonly used method for the preparation of HECs, which is suitable to not only oxides but also silicates, borides, carbides, silicide carbides, and sulfides [32,58,67,80,85,88,95,96,99,101,[109][110][111]. For example, Chen et al [90] High-entropy borides and carbides can also be synthesized using the solid state reaction method.…”

“…[106], who approximated configurational energies of HECs only by considering pairwise interactions, and analyzed the formation ability of rock-salt oxides by considering both the mean and the variance of configurational dependent energies. Similar descriptors as those of Sarker et al [64] and Pitike et al [106] in combination with redox mechanism were also adopted by Lun et al [67] to predict the formation ability of high-entropy battery cathodes. Zhang et al [111] developed a data-driven model to choose elements that may exhibit high possibility to form high-entropy sulfides.…”

“…Inspired by the pioneering work of Rost et al [29], most of the researches focus on the synthesis and property exploring of entropy stabilized oxides. Shortly, oxides with rock salt [21,29,[63][64][65][66][67], fluorite [38,60,[68][69][70][71], pyrochlore [36,37,[72][73][74][75], and spinel [80][81][82][83] structures were explored and fascinating properties brought by high-entropy effects have been reported. Gild et al [34] extended the material systems to ultrahigh temperature ceramics (UHTCs) by fabricating high-entropy borides with AlB 2 structure.…”

Magnetic properties of high entropy oxides

“…Many of the HEO crystal classes are known to afford stable Listorage possibilities, either via, conversion, intercalation or insertion. 26,[30][31][32]74,75 Systems like the spinels, are known to possess two electrochemical windows, one for intercalation and another for conversion. Utilizing the intercalation windows, in some of earlier studies magneto-ionic or electrochemically driven reversible tuning of magnetism in conventional spinels has been shown.…”

“…79 R-HEOs and S-HEOs, are known to be tolerant to reversible lithiation and delithiation, while layered HEOs are can reversibly accommodate both Li and Na. 26,27,31,32,75 Thus, stable reversible control of magnetism via the electrochemically-driven insertion/extraction of ions might be feasible. The chemical disorder can be of advantage to possibly making it easier to reach, conventionally inaccessible, magneto-electric free-energy minima.…”