High-Entropy Structure Design in Layered Transition Metal Dichalcogenides

Layered high-entropy compounds have been attracting a lot of attention in recent times due to their potential application in energy storage and conversion. Generally, an intra-layer scheme is widely used to realize the high-entropy structure by introducing multi-principal elements into the metal-atomic layers. Here, we propose an intercalation high-entropy scheme to realize the high-entropy structure in a series of layered transition metal dichalcogenides with a general chemical formula of MX2. Multi-principal metal elements are intercalated into the van-der-Waals gaps between MX2 slabs resulting in a series of (HEM)xMX2 compounds, in which HEM is high-entropy metals mainly composed of 3d transition metal elements such as Fe0.2Co0.2Cr0.2Ni0.2Mn0.2. Moreover, three kinds of 2D high-entropy magnetic lattices (a0 × a0, √3a0 × a0, √3a0 × √3a0) in the intercalated layers are found by tuning the intercalation content x. Significant differences in the effective moment and spin frustration among them are revealed. Furthermore, a multi-layered high-entropy structure is realized by a combination of intra-layer and intercalation schemes. The new intercalation high-entropy scheme and versatile 2D high-entropy structures reported in this work will reinforce the spirit on the exploration of new low-dimensional high-entropy systems for future applications.