Entropy Engineering of 2D Materials

Abstract Entropy, a measure of disorder or uncertainty in the thermodynamics system, has been widely used to confer desirable functions to alloys and ceramics. The incorporation of three or more principal elements into a single sublattice increases the entropy to medium and high levels, imparting these materials a mélange of advanced mechanical and catalytic properties. In particular, when scaling down the dimensionality of crystals from bulk to the 2D space, the interplay between entropy stabilization and quantum confinement offers enticing opportunities for exploring new fundamental science and applications, since the structural ordering, phase stability, and local electronic states of these distorted 2D materials get significantly reshaped. During the last few years, the large family of high‐entropy 2D materials is rapidly expanding to host MXenes, hydrotalcites, chalcogenides, metal‐organic frameworks (MOFs), and many other uncharted members. Here, the recent advances in this dynamic field are reviewed, elucidating the influence of entropy on the fundamental properties and underlying elementary mechanisms of 2D materials. In particular, their structure‐property relationships resulting from theoretical predictions and experimental findings are discussed. Furthermore, an outlook on the key challenges and opportunities of such an emerging field of 2D materials is also provided.