Atomic-Level Precision Synthesis and Dynamic Structure-Property Relationships of High-Entropy Nanomaterials: Advances, Challenges, and Perspectives

Abstract

High-entropy nanomaterials, which integrate five or more principal elements in equimolar or near-equimolar ratios into a single crystal lattice, have demonstrated immense potential in fields such as catalysis, energy storage, and conversion. This potential arises from their unique physicochemical properties, including the high-entropy effect, severe lattice distortion, sluggish diffusion kinetics, and the cocktail effect. Nevertheless, achieving precise synthesis and structural regulation at the atomic level remains a formidable challenge. Key obstacles include realizing atomic-scale homogeneous mixing of multiple elements, managing complex dynamic structural evolution, ensuring stability under non-equilibrium conditions, overcoming limitations in characterization resolution, addressing the challenges in scaling up synthesis techniques, and bridging the gap between theoretical predictions and experimental validation. This review systematically summarizes the critical scientific and technological issues associated with the atomic-level processing of high-entropy nanomaterials. It focuses on recent progress in advanced synthesis strategies, such as ultrafast high-temperature synthesis, molecular precursor design, machine learning-assisted composition screening, and interface engineering-employed to achieve precise structural control and performance optimization. Concurrently, the essential role of sophisticated characterization techniques in resolving complex structures is discussed. Finally, we outline future research directions, encompassing dynamic structure analysis, closed-loop intelligent synthesis and cross-scale interface design, with the aim of advancing their translation from fundamental research to industrial applications.