The elemental pegging effect in locally ordered nanocrystallites of high-entropy oxide enables superior lithium storage.

ABSTRACT

High-entropy oxides (HEOs) can be well suited for lithium-ion battery anodes because of their multi-principal synergistic effect and good stability. The appropriate selection and combination of elements play a crucial role in designing conversion-type anode materials with outstanding electrochemical performance. In this study, we have successfully built a single-phase spinel-structured HEO material of (Mn0.23Fe0.23Co0.22Cr0.19Zn0.13)3O4 (HEO-MFCCZ). When the HEO-MFCCZ materials transform into a coexisting state of amorphous and nanocrystalline structures during the cycling process, the inert Zn element can initiate a pegging effect, causing enhanced stability. The transition also introduces many defect sites, effectively reducing the potential barrier for ion transport and accelerating ion transport. The increased electronic and ionic conductivities and pseudocapacitive contribution significantly enhance the rate performance. As a result, a unique and practical approach is provided for developing anode materials for lithium-ion batteries.