Key Takeaways & Executive Findings
- •• Strategic heterostructure design creates electrified interfaces that induce a fully ionized depletion region and built-in electric field, enhancing Li affinity and promoting uniform current distribution for stable Li deposition. • The SnP0.94/CoP heterostructure enables in situ conversion to a mixed ionic/electronic conductor (MEIC) during cycling, ensuring long-term stability of the modulation layer. • SCP@Li symmetric cells achieve low overpotential for 750 cycles at 5 mA cm−2, demonstrating excellent cycling stability. • LiFePO4//SCP@Li full cells show imperceptible capacity decay of 0.03% per cycle over 800 cycles at 0.5 C, highlighting practical applicability.
Abstract
Regulating the nucleation and growth of Li metal is crucial for achieving stable high-energy-density Li metal batteries (LMBs) without dendritic Li growth, severe volume expansion, and “dead Li” accumulation. Herein, we present a modulation layer composed of porous SnP0.94/CoP p-n heterojunction particles (SCP), synthesized applying the Kirkendall effect. The unique heterointerfaces in the SCP induce a fully ionized depletion region and built-in electric field. This provides strong Li affinity, additional adsorption sites, and facilitated electron transfer, thereby guiding dendrite-free Li nucleation/growth with a low Li deposition overpotential. Moreover, the strategic design of the SCP, accounting for its reaction with Li, yields electronically conductive Co, lithiophilic Li–Sn alloy, and ionic conductive Li3P during progressive cycles. The mixed electronic and ionic conductor (MEIC) ensure the long-term stability of the SCP modulation layer. With this layer, the SCP@Li symmetric cell maintains a low overpotential for 750 cycles even at a high current density of 5 mA cm−2. Additionally, the LiFePO4//SCP@Li full cell achieves an imperceptible capacity decay of 0.03% per cycle for 800 cycles at 0.5 C. This study provides insight into MEIC heterostructures for high-performance LMBs.
1. Introduction
With the increase in global focus on environmental sustainability, secondary battery technology has advanced rapidly [1]. In addition, the growing demand for energy storage systems with higher energy densities (impelled by the rapid expansion of electric vehicles and consumer electronics markets) emphasizes the necessity of developing next-generation energy storage systems that surpass commercialized Li-ion batteries (LIBs) [2, 3]. Among the various candidates, lithium metal batteries (LMBs) constructed with Li metal anodes (LMAs) are widely considered as potential successors to LIBs for near-future energy markets because of their high theoretical capacity (3860 mAh g−1), low redox potential (−3.04 V vs. standard hydrogen electrode (SHE)), and low gravimetric density (0.59 g cm−3) [4, 5]. Nonetheless, the practical utilization of LMBs is impeded by persistent technical issues. The “hostless” LMAs with high reactivity can result in non-uniform Li-ion flux and irregular Li tip formation, which intensify the local charge density and electric field (called “tip effect”) [6]. Because the generated Li tips tend to evolve into Li dendrites, LMAs typically undergo infinite volume expansion and substantial mechanical stress, leading to damage the naturally formed solid electrolyte interphase (SEI) and the formation of inactive “dead” Li [7]. This mainly contributes to the continual consumption of organic electrolytes, degradation of electrochemical performance (particularly, the Coulombic efficiency (CE) and capacity decay), and safety hazard [8, 9]. Therefore, innovative approaches to stabilizing LMAs against dendrite formation and undesirable side reactions are essential for high-performance and safe LMB fabrication.
In response to the aforementioned challenges, numerous effective approaches have been proposed to mitigate the rambling growth of Li dendrites and side reactions, such as, adjusting the electrolyte composition [10, 11], introducing a modified separator [12], designing of 3D host/current collector [13, 14], adopting durable solid-state electrolytes [15, 16] and interfacial engineering of Li surfaces. Fine-tuning the electrolyte composition by adding functional additives (e.g., LiNO3 [17], fluoroethylene carbonate [18], and heptafluorobutyrylimidazole [19]) can regulate the chemical composition and structure of the SEI. This ensures its relative stability in the short term. However, these additives are gradually consumed, resulting in the collapse of the SEI and its accumulation during the prolonged cycling of LMBs because of the high reactivity of Li [20]. Based on Sand’s time t
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Jung Been Park, Changhoon Choi, Min Sang Kim, Hyeongbeom Kang, Eunji Kwon, Seungho Yu, Dong-Wan Kim (2025). Designing Metal Phosphide Solid-Electrolyte Interphase for Stable Lithium Metal Batteries Through Electrified Interface Optimization and Synergistic Conversion. Nano-Micro Letters. https://doi.org/10.1007/s40820-025-01813-1
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Frequently Asked Questions
What is the main challenge in lithium metal batteries that this study addresses?
The main challenge is the uncontrolled growth of lithium dendrites, which leads to low Coulombic efficiency, safety hazards, and short cycle life. This study addresses it by designing a metal phosphide solid-electrolyte interphase with electrified interfaces to guide uniform lithium deposition.
The heterostructure creates a built-in electric field and fully ionized depletion region, enhancing lithium affinity and promoting uniform current distribution. During cycling, it converts into a mixed ionic/electronic conductor (MEIC) that ensures long-term stability, resulting in dendrite-free lithium deposition and extended cycle life.
What are the key experimental results of the SCP@Li symmetric cell?
The SCP@Li symmetric cell maintains a low overpotential for 750 cycles at a high current density of 5 mA cm−2, demonstrating excellent cycling stability and low polarization.
What is the significance of the full cell performance in this study?
The LiFePO4//SCP@Li full cell achieves an imperceptible capacity decay of 0.03% per cycle over 800 cycles at 0.5 C, indicating high capacity retention and practical applicability for high-energy-density batteries.
What is the role of the Kirkendall effect in synthesizing the SCP particles?
The Kirkendall effect is utilized to synthesize porous SnP0.94/CoP p-n heterojunction particles, which provide unique heterointerfaces that induce the desired electrified interface and built-in electric field for improved lithium deposition behavior.
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