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Vol. 17 (2025)

Designing Metal Phosphide Solid-Electrolyte Interphase for Stable Lithium Metal Batteries Through Electrified Interface Optimization and Synergistic Conversion

https://doi.org/10.1007/s40820-025-01813-1
Jung Been Park
School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 02841, Republic of Korea
Changhoon Choi
Department of Materials Science and Engineering, SungShin Women’s University, Seoul 01133, Republic of Korea
Min Sang Kim
School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 02841, Republic of Korea
Hyeongbeom Kang
School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 02841, Republic of Korea
Eunji Kwon
Energy Storage Research Center, Korea Institute of Science and Technology, 5, Hwarang‑ro 14‑gil, Seongbuk‑gu, Seoul 02792, Republic of Korea
Seungho Yu
Energy Storage Research Center, Korea Institute of Science and Technology, 5, Hwarang‑ro 14‑gil, Seongbuk‑gu, Seoul 02792, Republic of Korea
Dong‑Wan Kim
School of Civil, Environmental, and Architectural Engineering, Korea University, Seoul 02841, Republic of Korea

Corresponding Author: Dong‑Wan Kim

dwkim1@korea.ac.kr

Nano-Micro Letters, Vol. 17 (2025), Article Number: 315

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.


Highlights:
1 Through strategic heterostructure design, it is possible to create electrified interfaces that induce the formation of a fully ionized depletion region and a built-in electric field.
2 These electrified interfaces enhance Li affinity and promote uniform current distribution, leading to stable Li deposition behavior.
3 Owing to intentional design, SnP0.94/CoP heterostructure enables in situ conversion to a mixed ionic/electronic conductor during cycling, ensuring the long lifespan.

Keywords

Li metal batteries Heterostructures In situ reactions Dendrite-free anodes Mixed ionic/electronic conductors
Park, Jung Been, Changhoon Choi, Min Sang Kim, Hyeongbeom Kang, Eunji Kwon, Seungho Yu, and 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 17 (June):315. https://doi.org/10.1007/s40820-025-01813-1.
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