Modification of 2D materials using MoS2 as a model for investigating the Al-storage properties of diverse crystal facets

Abstract

Research on aluminum batteries (ABs) is becoming a hotspot due to their low cost, high specific capacity, and high safety. However, the limited charge-storage capacity of cathodes has impeded the development of ABs. In this work, a novel modification strategy for 2D materials was applied to a MoS₂ model to obtain a S–MoS₂ cathode with large interlayer spacing and specific surface area, and its intrinsic energy-storage mechanisms were thoroughly studied. The experimental results verify that S–MoS₂ possesses fast reaction kinetics and outstanding electrochemical energy-storage performance. Notably, the intrinsic interactions of all potential active surfaces in MoS₂ with Al³⁺ and AlCl₄⁻ have been investigated comprehensively through DFT simulations for the first time. Compared with the (001) and interlayer surfaces, the lateral stacking (100) facet has stronger reactivity and adsorption stability. These in-depth insights gained from this work may contribute to the further design of 2D materials in a wide field.