Unveiling the abnormal capacity rising mechanism of MoS2 anode during long-term cycling for sodium-ion batteries

Abstract

Transition metal sulfides are considered as one of the most potential anode materials in sodium-ion batteries due to their high capacity, low cost, and rich resources. Among plenty of options, molybdenum sulfide (MoS₂) has been the focus of research due to the graphene-like layered structure and unique electrochemical properties. Importantly, an abnormal capacity increase phenomenon was observed in the MoS₂ anode of sodium-ion batteries, but the mechanisms involved are still unclear. In this study, by analyzing the composition and structure of the material after a different number of cycles, we confirmed that the (002) plane shows a significant expansion of the interlayer spacing after the sodium ion insertion process and a phase transformation from the hexagonal phase MoS₂ (2H-MoS₂) to the trigonal phase MoS₂ (1T-MoS₂). Moreover, the ratio of 1T-MoS₂ presented an increasing trend during cycling. The dual-phase co-existence leads to enhanced electrical conductivity, higher Na affinity, and higher Na⁺ mobility, thus increasing the capacity. Our work provides a new perspective on the anomalous electrochemical behavior of sulfide anodes during long-term cycling.