Lithium Storage Mechanisms and Electrochemical Behavior of a Molybdenum
Disulfide Nanoparticle Anode
Abstract
This study investigates the electrochemical behavior of molybdenum
disulfide (MoS2) as an anode in Li-ion batteries, focusing on the extra
capacity phenomenon. Employing advanced characterization methods such as
in situ and ex situ X-ray diffraction, Raman spectroscopy, X-ray
photoelectron spectroscopy, and transmission electron microscopy, the
research unravels the complex structural and chemical evolution of MoS2
throughout its cycling. A key discovery is the identification of a
unique Li intercalation mechanism in MoS2, leading to the formation of
reversible LixMoS2 phases that contribute to the extra capacity of the
MoS2 electrode. Density function theory calculations suggest the
potential for overlithiation in MoS2, predicting Li5MoS2 as the most
energetically favorable phase within the lithiation-delithiation
process. Additionally, the formation of a Li-rich phase on the surface
of Li4MoS2 is considered energetically advantageous. After the first
discharge, the battery system engages in two main reactions. One
involves operation as a Li-sulfur battery within the carbonate
electrolyte, and the other is the reversible intercalation and
deintercalation of Li in LixMoS2. The latter reaction contributes to the
extra capacity of the battery. The incorporation of reduced graphene
oxide as a conductive additive in MoS2 electrodes notably improves their
rate capability and cycling stability.