Key Takeaways & Executive Findings
- •• First-ever fabrication of anode-free all-solid-state battery (AFASSB) structure using a MoS2 sacrificial layer. • MoS2 sacrificial layer reduces Li nucleation overpotential and enables favorable Li formation via Li2S and Mo interlayer. • AFASSB full cells with LiNi0.6Co0.2Mn0.2O2 cathodes show superior cycling stability and enhanced capacity compared to SUS. • Optimal MoS2 thickness yields 1.18-fold increase in initial discharge capacity and sevenfold improvement in capacity retention.
Abstract
Anode-free all-solid-state batteries (AFASSBs) are potential candidates for next-generation electric mobility devices that offer superior energy density and stability by eliminating Li from the anode. However, despite its potential to stabilize the interface between sulfide solid electrolytes (SEs) and anode-free current collectors (CCs) efficiently, a controllable approach to incorporating MoS2 into AFASSBs has not yet been found. Herein, we propose a strategy for stabilizing the interface of Li-free all-solid-state batteries using controllable MoS2 sacrificial thin films. MoS2 was controllably grown on CCs by metal–organic chemical vapor deposition, and the MoS2 sacrificial layer in contact with the SEs formed an interlayer composed of Mo metal and Li2S through a conversion reaction. In the AFASSBs with MoS2, Mo significantly reduces the nucleation overpotential of Li, which results in uniform Li plating. In addition, MoS2-based Li2S facilitates the formation of a uniform and robust SE interface, thereby enhancing the stability of AFASSBs. Based on these advantages, cells fabricated with MoS2 exhibited better performance as both asymmetrical and full cells with LiNi0.6Co0.2Mn0.2O2 cathodes than did cells without MoS2. Moreover, the cell performance was affected by the MoS2 size, and full cells having an optimal MoS2 thickness demonstrated a 1.18-fold increase in the initial discharge capacity and a sevenfold improvement in capacity retention relative to SUS CCs. This study offers a promising path for exploiting the full potential of MoS2 for interface stabilization and efficient AFASSB applications.
1. Introduction
Anode-free all-solid-state batteries (AFASSBs) are promising for next-generation electric mobility due to their high energy density and safety, but they face challenges in achieving uniform lithium deposition and stable interfaces. To address this, various functional layers have been explored to improve the uniformity of initial lithium deposition and battery stability. For instance, the Samsung Group reported that Ag nanoparticles in Ag-C composite layers provide Li nucleation sites and promote uniform Li plating onto current collectors (CCs) in all-solid-state batteries (ASSBs). Subsequent studies have investigated coating various Li-friendly metals onto CCs as functional layers, such as Mg and Ag-In alloys, which exhibit low reaction barriers with Li and facilitate reversible Li plating and stripping. However, these lithiophilic metals and their composites have limitations in industrial applications due to high material costs, fire-related instability, and relatively thick layers. Moreover, a comprehensive approach that integrates functional layers with surface morphology modifications for effective AFASSB operation has yet to be reported.
Transition metal dichalcogenides (TMDs) have attracted attention due to their earth abundance, low cost, exceptional electronic properties, and energy-harvesting performance. MoS2, a typical TMD, is considered an ideal material for constructing high-quality Li-protective layers due to its advantageous properties. Recent studies have revealed that MoS2 is an excellent Li+ conductor, making it a promising candidate for stabilizing the interface in Li-free batteries. In this work, we propose a strategy using controllable MoS2 sacrificial thin films grown on CCs by metal–organic chemical vapor deposition. The MoS2 layer reacts with sulfide solid electrolytes to form an interlayer of Mo metal and Li2S, which reduces nucleation overpotential and promotes uniform Li plating, thereby enhancing the performance and stability of AFASSBs.
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Dong-Bum Seo, Dohun Kim, Mee-Ree Kim, Jimin Kwon, Hyeong Jun Kook, Saewon Kang, Soonmin Yim, Sun Sook Lee, Dong Ok Shin, Ki-Seok An, Sangbaek Park (2025). Tailoring Artificial Solid Electrolyte Interphase via MoS2 Sacrificial Thin Film for Li-Free All-Solid-State Batteries. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01729-w
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Frequently Asked Questions
What is an anode-free all-solid-state battery (AFASSB)?
An AFASSB is a type of all-solid-state battery that eliminates the lithium metal anode, using a current collector as the anode substrate. This design increases energy density and safety by reducing weight and volume, but requires careful interface engineering to achieve uniform lithium plating and stripping.
How does the MoS2 sacrificial layer improve battery performance?
The MoS2 sacrificial layer reacts with sulfide solid electrolytes to form an interlayer composed of Mo metal and Li2S. Mo reduces the nucleation overpotential of lithium, promoting uniform lithium plating, while Li2S helps form a stable solid electrolyte interphase, enhancing cycling stability and capacity retention.
What are the key advantages of using MoS2 over other lithiophilic metals?
MoS2 is earth-abundant, low-cost, and can be controllably deposited as a thin film. It provides dual benefits: the Mo metal improves lithium nucleation, and the Li2S enhances interface stability. This leads to better performance compared to conventional metals like Ag or Mg, which may be more expensive or less effective.
What is the significance of the optimal MoS2 thickness?
The study found that the performance of AFASSBs is affected by the MoS2 thickness. An optimal thickness maximizes the benefits, resulting in a 1.18-fold increase in initial discharge capacity and a sevenfold improvement in capacity retention compared to cells without MoS2, highlighting the importance of precise control.
What are the potential applications of this technology?
This technology could be applied in next-generation electric vehicles and portable electronics, where high energy density and safety are critical. The use of MoS2 sacrificial layers offers a scalable and cost-effective approach to improve the performance of anode-free all-solid-state batteries.
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