RÉSUMÉ
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 FeMnNiVZnPS3. Aperiodic stacking is found in FeMnNiVZnPS3 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 FeMnNiVZnPS3. 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 FeMnNiVZnPS3 demonstrates superior ion-diffusion coefficients of 10-9.7-10-8.3 cm2 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.
RÉSUMÉ
The hexagonal WO3 polymorph, h-WO3, has attracted attention due to its interatomic channels, allowing for a greater degree of intercalation compared to other WO3 polymorphs. Our research group has previously demonstrated h-WO3 to be a highly sensitive gas sensing material for a flu biomarker, isoprene. In this work, the gas sensing performance of this polymorph has been further investigated in two distinct configurations of the material produced by different processing routes. The first sample was synthesized using Na2WO4·2H2O and showed (100) faceting. The second sample was synthesized using WCl6 and showed (001) faceting. The gas sensing response of the nanostructured films deposited using the (100) textured h-WO3 sample 1 had a higher response to acetone at 350 °C. The (001) textured h-WO3 sample 2 favored isoprene at 350 °C. The selectivity of the latter to isoprene is explained in terms of the dangling bonds present on the (001) facets. The tungsten and oxygen dangling bonds present on the (001) plane favor the adsorption of the isoprene molecule over that of the acetone molecule due to the oxygen containing dipole present in the acetone molecule.