Gradient-Engineered Ultra-Thin Lithium Metal Anodes with a Li–Si–N Alloy-Based Lithiophilic Current Collector Interphase

Jihyeon Kang; Mihee Park; Jueun Kim; Jihan Park; Byungsuk Lee; Jinhong Lee; Pilgun Oh; Kyujung Kim; Jun-Woo Park; Minjoon Park

doi:10.1002/eem2.70154

Energy & Environmental Materials ›› 2026, Vol. 9 ›› Issue (2) :e70154 DOI: 10.1002/eem2.70154

Research Article

Gradient-Engineered Ultra-Thin Lithium Metal Anodes with a Li–Si–N Alloy-Based Lithiophilic Current Collector Interphase

Jihyeon Kang ¹^,²^,³
, Mihee Park ⁴^,⁵
, Jueun Kim ¹^,²^,³
, Jihan Park ¹^,²^,³
, Byungsuk Lee ⁴^,⁵
, Jinhong Lee ⁶
, Pilgun Oh ⁷
, Kyujung Kim ⁴^,⁵
, Jun-Woo Park ⁸^,⁹
, Minjoon Park ¹^,²^,³

Author information +

¹. Department of Nanoenergy Engineering, Pusan National University, 50, Busan daehak-ro 63 beon-gil 2, Geumjeong-gu, Busan, 46241 Korea

². Department of Nano Fusion Technology, Pusan National University, Busandaehak-ro 63beon-gil 2, Geumjeong-gu, Busan, 46241 Korea

³. Research Center of Energy Convergence Technology, Pusan National University, Busandaehak-ro 63beon-gil 2, Geumjeong-gu, Busan, 46241 Korea

⁴. Department of Cogno-Mechatronics Engineering, College of Nanoscience and Nanotechnology, Pusan National University, Busan, 46241 Korea

⁵. Department of Optics and Mechatronics Engineering, College of Nanoscience and Nanotechnology, Pusan National University, Busan, 46241 Korea

⁶. School of Chemical Engineering, Pusan National University, Busan, 46241 Korea

⁷. Department of Smart Green Technology Engineering, Department of Nanotechnology Engineering, Pukyong National University, Busan, 48547 Korea

⁸. Next Generation Battery Research Center, Korea Electrotechnology Research Institute (KERI), Changwon-si, Gyeongsangnam-do, 51543 Korea

⁹. Department of Electro-Functionality Materials Engineering, University of Science and Technology (UST), Daejeon, 34113 Korea

poh@pknu.ac.kr

k.kim@pusan.ac.kr

parkjw@keri.re.kr

mjpark@pusan.ac.kr

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Abstract

Li metal anodes, with high theoretical capacity (3860 mAh g⁻¹) and low redox potential, are promising for high-capacity rechargeable batteries. Especially, ultra-thin Li metal anodes can improve energy density and minimize lithium excess. However, their poor processability leads to non-uniform Li layers and unstable plating/stripping behavior. In this study, we present a current collector interphase (CCI)-based strategy using a Cu foil coated with a lithiophilic Si₃N₄ layer, followed by molten Li dip-coating to form around 20 μm Li layer. Furthermore, the scalable dip-coating method, compatibility with large-area current collectors (up to 100 cm²), and stable cycling in pouch cells demonstrate the practical viability of the proposed SNLMA design for commercial lithium metal batteries. During the process, an in-situ Li–Si–N alloy gradient interphase forms at the interface, enhancing wettability and mechanical integrity. This unique gradient CCI provides synergistic lithiophilicity and structural stability, enabling high-performance Li metal batteries. The resulting Li_xSi_y and Li_xN_y phases reduce nucleation barriers and enable uniform Li deposition. As a result, the Si₃N₄–Li anode paired with a high-loading LCO cathode (22 mg cm⁻²) achieved 83% capacity retention after 100 cycles. This work offers a scalable and practical CCI design for next-generation Li metal batteries.

Keywords

current collector interphase / lithium / lithium metal anode / lithium metal battery / silicon nitride

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Jihyeon Kang, Mihee Park, Jueun Kim, Jihan Park, Byungsuk Lee, Jinhong Lee, Pilgun Oh, Kyujung Kim, Jun-Woo Park, Minjoon Park. Gradient-Engineered Ultra-Thin Lithium Metal Anodes with a Li–Si–N Alloy-Based Lithiophilic Current Collector Interphase. Energy & Environmental Materials, 2026, 9 (2) : e70154 DOI:10.1002/eem2.70154

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