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<p>Anode-free lithium-ion batteries (AFLBs) and lithium metal batteries (LMBs), which offer exceptionally high volumetric and gravimetric energy densities, are considered promising candidates for next-generation energy storage systems. However, their practical application remains limited by poor cycling stability, primarily resulting from low Coulombic efficiency (CE) caused by non-uniform plating/deplating behavior at the anode. In this study, a 15&#xa0;nm-thick Zr-based metallic glass thin film (Zr<sub>53</sub>Cu<sub>31</sub>Ni<sub>11</sub>Al<sub>5</sub>, denoted as 15Zr-MG) was deposited onto a polypropylene separator via magnetron sputtering. The 15Zr-coated separator (15Zr-S) exhibited enhanced electrolyte wettability and improved electrochemical performance. Electrochemical impedance spectroscopy (EIS) analysis revealed that both the solid electrolyte interphase resistance (R<sub>SEI</sub>) and charge transfer resistance (R<sub>ct</sub>) were reduced in half cells and symmetric cells using the 15Zr-S. Overpotential analysis showed a lower nucleation overpotential (η<sub>n</sub>) and a reduced crystallization overpotential (η<sub>c</sub>), confirming more uniform Li deposition. Furthermore, the symmetric cell containing the 15Zr-S maintained low polarization below 0.02&#xa0;V for over 500&#xa0;h, indicating smooth, stable, and reversible Li plating/stripping behavior. Scanning electron microscopy confirmed the formation of horizontally aligned and uniform Li deposits on the 15Zr-S. Consequently, high initial discharge capacities of 140.7 mAh g<sup>− 1</sup> and 103.0 mAh g<sup>− 1</sup> were obtained for AFLBs and LMBs, respectively. The LMBs also exhibited an increased discharge capacity of 108.9 mAh g<sup>− 1</sup> after 400 cycles, demonstrating enhanced cycling performance. These results confirm that 15Zr-MG coating effectively regulates Li⁺ flux, suppresses dendrite growth, and significantly improves the electrochemical performance of both AFLBs and LMBs.</p>

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Zr-based metallic glass-coated separator for stable anode-free lithium-Ion batteries and lithium metal batteries

  • 期刊论文

  • 发表日期：

    2026年2月19日

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  • Woon-Hyun Jo,
  • Ga Yeon Lee,
  • Suk Jun Kim

摘要

Anode-free lithium-ion batteries (AFLBs) and lithium metal batteries (LMBs), which offer exceptionally high volumetric and gravimetric energy densities, are considered promising candidates for next-generation energy storage systems. However, their practical application remains limited by poor cycling stability, primarily resulting from low Coulombic efficiency (CE) caused by non-uniform plating/deplating behavior at the anode. In this study, a 15 nm-thick Zr-based metallic glass thin film (Zr53Cu31Ni11Al5, denoted as 15Zr-MG) was deposited onto a polypropylene separator via magnetron sputtering. The 15Zr-coated separator (15Zr-S) exhibited enhanced electrolyte wettability and improved electrochemical performance. Electrochemical impedance spectroscopy (EIS) analysis revealed that both the solid electrolyte interphase resistance (RSEI) and charge transfer resistance (Rct) were reduced in half cells and symmetric cells using the 15Zr-S. Overpotential analysis showed a lower nucleation overpotential (ηn) and a reduced crystallization overpotential (ηc), confirming more uniform Li deposition. Furthermore, the symmetric cell containing the 15Zr-S maintained low polarization below 0.02 V for over 500 h, indicating smooth, stable, and reversible Li plating/stripping behavior. Scanning electron microscopy confirmed the formation of horizontally aligned and uniform Li deposits on the 15Zr-S. Consequently, high initial discharge capacities of 140.7 mAh g− 1 and 103.0 mAh g− 1 were obtained for AFLBs and LMBs, respectively. The LMBs also exhibited an increased discharge capacity of 108.9 mAh g− 1 after 400 cycles, demonstrating enhanced cycling performance. These results confirm that 15Zr-MG coating effectively regulates Li⁺ flux, suppresses dendrite growth, and significantly improves the electrochemical performance of both AFLBs and LMBs.