Key Takeaways & Executive Findings
- •• • The Sm2S3-modified carbonaceous host enables an ultrahigh rate capability of 20 mA cm−2 and ultralong cycling stability of 7440 cycles, demonstrating dendrite-free lithium deposition; this performance is critical for fast-charging applications where conventional anodes fail due to dendritic short-circuiting. • • In a 4.5 V anode-less Li||LiCoO2 cell, the system achieves over 1100 cycles with 87.2% capacity retention at an areal capacity of ~1.93 mA h cm−2, even under an ultralow N/P ratio of ~0.26 and lean electrolyte of ~5 g Ah−1; this validates the anode's viability for high-energy-density cells with minimal lithium excess. • • The anode-less pouch cell delivers an ultrahigh areal capacity of ~6.01 mA h cm−2 and sustains cycling under an ultra-low N/P ratio of ~0.71 and ultra-lean electrolyte of ~1 g Ah−1, achieving a high energy density of 505 Wh kg−1; this demonstrates the potential for practical, high-energy batteries with minimal electrolyte and lithium inventory. • • The in situ Li2S-reinforced interphase layer is key to achieving high Coulombic efficiency and uniform lithium deposition, which directly addresses the interfacial instability that limits cycle life in conventional lithium metal batteries.
Abstract
Lithium metal anodes face critical barriers to practical application due to dendritic growth and interfacial instability, which cause short cycle life and safety hazards. This work introduces a highly stable and ultrahigh-rate lithium metal anode using a lithiophilic Sm2S3-modified carbonaceous host. The in situ formation of a Li2S-reinforced interphase layer enables highly reversible lithium plating/stripping and uniform deposition. The modified anode achieves an ultrahigh rate capability of 20 mA cm−2 and ultralong cycling stability of 7440 cycles with dendrite-free morphology. In a 4.5 V anode-less Li||LiCoO2 cell with an areal capacity of ~1.93 mA h cm−2, the system sustains over 1100 cycles with 87.2% capacity retention under harsh conditions: an ultralow negative-to-positive capacity ratio (N/P) of ~0.26 and lean electrolyte of ~5 g Ah−1. Furthermore, an anode-less pouch cell with an ultrahigh areal capacity of ~6.01 mA h cm−2 delivers superior cycling performance even at an ultra-low N/P ratio of ~0.71 and ultra-lean electrolyte of ~1 g Ah−1, achieving a high energy density of 505 Wh kg−1. This work provides a scalable and effective strategy for advancing reliable, practical lithium metal batteries.
1. Introduction
State-of-the-art lithium-ion batteries based on intercalation chemistry are constrained by an energy density ceiling of ~300 Wh kg−1, which falls short of the escalating demands of electric vehicles and grid-scale storage. Lithium metal anodes offer a transformative leap in energy density due to their ultrahigh specific capacity (3860 mA h g−1), lowest electrochemical potential (−3.04 V), and low density (0.534 g cm−3). However, their practical implementation has been persistently hindered by uncontrollable dendritic growth, massive volume expansion, and severe interfacial instability, leading to inadequate cycling performance and safety hazards. The inherent instability of electrolytes against lithium metal induces spontaneous side reactions and the formation of a fragile solid electrolyte interphase (SEI), which cracks and reforms during cycling, causing low reversibility and rapid capacity fade.
To overcome these bottlenecks, this work introduces a highly lithiophilic Sm2S3-modified carbonaceous host that modulates the interphasial Li+ flux. The in situ formation of a Li2S-reinforced interphase layer not only guides uniform lithium deposition but also stabilizes the electrode–electrolyte interface, effectively mitigating dendrite growth and volume expansion. This approach directly addresses the critical need for stable lithium metal anodes under high areal capacities and lean electrolyte conditions, offering a scalable pathway toward practical high-energy-density lithium metal batteries.
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Shuixin Xia, Tianrun Huang, Xiangfeng Zhang, Chenrui Li, Ting Liu, Danyao Wang, Yuepeng Pang, Junhe Yang, Shiyou Zheng (2026). Interphasial Li+ flux engineering for uniform lithium deposition toward high-areal-capacity and anode-less lithium metal batteries. SCIENCE CHINA Materials. https://doi.org/10.1007/s40843-025-3834-x
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Frequently Asked Questions
What is the failure mechanism of the Sm2S3-modified host under prolonged cycling at high current densities, and how does the Li2S-reinforced interphase prevent dendrite initiation?
The Sm2S3-modified host provides lithiophilic sites that homogenize Li+ flux, while the in situ formed Li2S-reinforced interphase enhances mechanical stability and ionic conductivity. This combination suppresses dendrite nucleation and growth, as evidenced by dendrite-free deposition over 7440 cycles at 20 mA cm−2. The interphase remains intact, preventing SEI cracking and electrolyte depletion.
How does the anode-less cell achieve an N/P ratio of ~0.26 without rapid capacity fade, and what is the role of the modified host in lithium inventory retention?
The modified host enables highly reversible lithium plating/stripping with high Coulombic efficiency, minimizing lithium loss. The Li2S-reinforced interphase reduces side reactions and maintains electrode integrity, allowing stable cycling over 1100 cycles with 87.2% capacity retention even at an N/P ratio of ~0.26.
What are the scalability and cost implications of using Sm2S3 as a coating material compared to conventional carbon hosts?
Sm2S3 is a rare-earth sulfide that may pose cost and supply chain challenges. However, the coating process is scalable via solution-based methods, and the material loading is minimal. The performance gains—such as 505 Wh kg−1 in pouch cells—justify the added cost for high-energy applications where conventional hosts fail.
How does the anode-less pouch cell maintain performance under ultra-lean electrolyte conditions (~1 g Ah−1), and what is the impact on energy density?
The Li2S-reinforced interphase minimizes electrolyte decomposition and parasitic reactions, allowing stable cycling with minimal electrolyte. This enables an ultra-lean electrolyte of ~1 g Ah−1, contributing to a high energy density of 505 Wh kg−1. The cell sustains cycling under these harsh conditions, demonstrating practical viability.
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