High-entropy materials (HEMs) are extremely popular for electrochemical energy storage nowadays. However, the detailed effects of four core factors of high entropy on the electrochemical properties of HEMs are still unclear. Here, a high-entropy LaCePrNdNbO (HE-LaNbO) oxide is prepared through multiple rare-metal-ion substitution in LaNbO, and uses HE-LaNbO as a model material to systematically study the effects of the four core factors of high entropy on electrochemical energy-storage materials. The high-entropy effect lowers the calcination temperature for obtaining pure HE-LaNbO. The lattice distortion in HE-LaNbO leads to its decreased unit-cell-volume variations, which benefits its cyclability. Based on the restrained diffusion arising from the lattice distortion, the Li diffusivity of HE-LaNbO at room temperature (25 °C) is limited, which causes its lowered rate capability. However, the Li diffusivity of HE-LaNbO at high temperature (60 °C) becomes faster than that of LaNbO, which is attributed to the alleviated lattice distortion at the high-temperature, resulting in higher rate capability. The cocktail effects in HE-LaNbO enable its larger electronic conductivity, better electrochemical activity, more intensive Nb ↔ Nb redox reaction, and larger reversible capacity. The insight gained here can provide a guide for the rational design of new HEMs with good energy-storage properties.

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http://dx.doi.org/10.1002/advs.202411291DOI Listing

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