Stepwise Elemental Screening of High‐Entropy Oxides as Zero‐Strain and High‐Capacity Anode in LIBs

ABSTRACT High‐entropy oxides (HEOs) have attracted much attention as advanced anode materials for LIBs due to their potential for synergistic optimization of specific capacity, rate capability, and cycling stability, due to the multi‐component cocktail effect. However, due to the complexity of multi‐component systems and the lack of theoretical frameworks, the exploration of HEOs is costly and time‐consuming. This study proposes a stepwise element screening strategy centered on formation energy and lithium‐embedded volume change as core evaluation metrics, through data statistics of previous literature and materials calculations. A novel zero‐strain anode material (CoFeMnNiZnMgLi) 3 O 4 was predicted and prepared. Electrochemical tests and characterizations at lattice, particle, and electrode scales confirm the feasibility of the presented elemental screening. The well‐designed HEOs achieved a specific capacity of 890 mAh/g at 0.1 A/g and exhibited almost no capacity decay after 3000 cycles at 5 A/g. Meanwhile, its maximum c‐axis strain and volume change of the unit cell during Li + insertion//extraction are as low as ∼0.13% and ∼0.38%, respectively. Most importantly, the presented high‐efficiency approach based on an entropy‐mediated mechanism holds great promise for developing host materials for various ions with low‐strain and high‐capacity.