High‐Entropy Transition Metal Phosphorus Trichalcogenides for Rapid Sodium Ion Diffusion

Abstract High‐entropy strategies are regarded as a powerful means to enhance performance in energy storage fields. The improved properties are invariably ascribed to entropy stabilization or synergistic cocktail effect. Therefore, the manifested properties in such multicomponent materials are usually unpredictable. Elucidating the precise correlations between atomic structures and properties remains a challenge in high‐entropy materials (HEMs). Herein, atomic‐resolution scanning transmission electron microscopy annular dark field (STEM‐ADF) imaging and four dimensions (4D)‐STEM are combined to directly visualize atomic‐scale structural and electric information in high‐entropy FeMnNiVZnPS 3 . Aperiodic stacking is found in FeMnNiVZnPS 3 accompanied by high‐density strain soliton boundaries (SSBs). Theoretical calculation suggests that the formation of such structures is attributed to the imbalanced stress of distinct metal‐sulfur bonds in FeMnNiVZnPS 3 . Interestingly, the electric field concentrates along the two sides of SSBs and gradually diminishes toward the two‐dimensional (2D) plane to generate a unique electric field gradient, strongly promoting the ion‐diffusion rate. Accordingly, high‐entropy FeMnNiVZnPS 3 demonstrates superior ion‐diffusion coefficients of 10 −9.7 ‐10 −8.3 cm 2 s −1 and high‐rate performance (311.5 mAh g −1 at 30 A g −1 ). This work provides an alternative way for the atomic‐scale understanding and design of sophisticated HEMs, paving the way for property engineering in multi‐component materials.