Two Birds with One Stone: Prelithiated Two-Dimensional Nanohybrids as High-Performance Anode Materials for Lithium-Ion Batteries

Abstract

As an inexpensive and naturally abundant two-dimensional (2D) material, molybdenum disulfide (MoS2) exhibits a high Li-ion storage capacity along with a low volume expansion upon lithiation, rendering it an alternative anode material for lithium-ion batteries (LIBs). However, the challenge of using MoS2-based anodes is their intrinsically low electrical conductivity and unsatisfied cycle stability. To address the above issues, we have exploited a wet chemical technique and integrated MoS2 with highly conductive titanium carbide (Ti3C2) MXene to form a 2D nanohybrid. The binary hybrids were then subjected to an n-butyllithium (n-Buli) treatment to induce both MoS2 deep phase transition and MXene surface functionality modulation simultaneously. We observed a substantial increase in 1T-phase MoS2 content and a clear suppression of −F-containing functional groups in MXene due to the prelithiation process enabled by the n-Buli treatment. Such an approach not only increases the overall network conductivity but also improves Li-ion diffusion kinetics. As a result, the MoS2/Ti3C2 composite with n-Buli treatment delivered a high Li-ion storage capacity (540 mA h g–1 at 100 mA g–1), outstanding cycle stability (up to 300 cycles), and excellent rate capability. This work provides an effective strategy for the structure–property engineering of 2D materials and sheds light on the rational design of high-performance LIBs using 2D-based anode materials.

Advancements in Prelithiation Technology: Transforming Batteries from Li‐Shortage to Li‐Rich Systems

“…Reproduced with permission. [ 68 ] Copyright 2022, American Chemical Society. i) Schematic illustration of redox potential and structure of Flr‐Li, Bp‐Li, Naph‐Li, and Bu‐Li prelithiation reagents.…”

“…After Bu-Li treatment, the 1T-phase MoS 2 content of MoS 2 /MXene was increased while MXene containing ─F functional groups were suppressed, which facilitated the conductivity enhancement (Figure 7h). [68] Huang et al described a novel lithium 9,9-dimethylfluorene (Li-DiMF) lithiation reagent with a low redox potential of 0.22 V (vs Li/Li + ). The powerful Li-DiMF Reproduced with permission.…”

“…h) Schematic illustration of Bu-Li treatment for MoS 2 /MXene nanohybrid structures. Reproduced with permission [68]. Copyright 2022, American Chemical Society.…”

Li2SiF6 In Situ Embedded in an Amorphous SiO Matrix to Inhibit Volume Expansion during Prelithiation

“…At present, much research has been launched on prelithiation, mainly including chemical prelithiation, , electrochemical prelithiation, direct contact prelithiation, − and so on. Among them, chemical prelithiation mainly applies lithium-containing reactant additives with very strong reducing properties to approach the negative electrode, such as lithium biphenyl, − lithium naphthalene, lithium butyl, etc. The effect of rapid prelithiation can be achieved by regulating the redox potential of the prelithiation reagent.…”

Effect of intercalated molybdenum atoms on structure and electrochemical properties of Mo1+x S2 synthesized by hydrothermal method

“…Besides, the larger layer spacing of MoS 2 compared with that of graphite can effectively inhibit the volume expansion caused by the insertion of lithium ions [8,9].…”