  Van der Waals (vdW) heterostructures have attracted intense interest
worldwide as they offer several routes to design materials with novel features
and wide-ranging applications. Unfortunately, at present, vdW heterostructures
are restricted to a small number of stackable layers, due to the weak vdW
forces holding adjacent layers together. In this work, we report on
computational studies of a bulk vdW material consisting of alternating TiS2 and
TiSe2 (TSS) vertically arranged layers as a potential candidate for anode
applications. We use density functional theory (DFT) calculations and ab-initio
molecular dynamics (AIMD) simulations to explore the effect of high entropy on
several electrochemically relevant properties of the bulk heterostructure
(TSS-HS) by substituting Mo6+ and Al3+ at the transition metal site (Ti4+). We
also study the solvation shell formation at the electrode-electrolyte interface
(EEI) using AIMD to determine Li-coordination. Based on the properties computed
using DFT and AIMD we propose that high entropy TSS-HS (TSS-HE) might possess
improved electrochemical performance over standard TSS-HS. Factors that could
improve the performance of TSS-HE are 1) Less structural deformation, 2) Strong
bonding (Metal-Oxygen), 3) Better electron mobility, 4) Wider operational
voltage window, and 5) Faster Li-ion diffusion. Our observations suggest that
'high entropy' can be an effective strategy to design new anode materials for
improving electrochemical performance of Li-ion batteries.
