Mixed Enthalpy-Entropy Descriptor Guided Discovery of 2D High-Entropy Chalcogenides for Energy Applications*

Over the past few years, the discovery of high-entropy materials (HEMs) has sparked significant interest in condensed matter physics and materials science due to their potential for a wide range of applications. These materials have been of growing interest, but the design of HEMs faces daunting challenges, which have been recently overcome by the Mixed Enthalpy-Entropy Descriptor (MEED) that successfully predicted several experimentally reported HEMs from first principles. In this work, the MEED has been used to screen the materials space of 2D chalcogenides of metals (Hf, Nb, Mo, Ta, Ti, V, W, and Zr) in the 2H, 1T, and 1T' phases, comprising four, five, and six principal metal elements. Interestingly, MEED captures the structural aspects relevant to the synthesis of HEMs in their respective polymorphs, further showcasing its unique capability. Additionally, based on MEED predictions for 2D high-entropy chalcogenides, several top-candidate high-entropy tellurides have been successfully synthesized. Furthermore, the results indicate that these high-entropy tellurides, which can blend the combinatorial properties of HEMs with the large surface area of 2D materials, exhibit exceptional characteristics for applications in batteries and catalysis.