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<p>The intrinsic characteristics of the Li metal anode, particularly its ultra-high specific capacity (3860&#xa0;mAh&#xa0;g<sup>−1</sup>) and low redox potential (−3.04&#xa0;V vs. SHE), theoretically make it ideal for high-rate charge/discharge operations. However, the high Li self-diffusion barrier causes uncontrolled plating/stripping dynamics and severe volume fluctuations, hindering stable performance at elevated current densities. In this study, we introduced an artificial solid-electrolyte interphase (ASEI) engineered with a bilayer that transcends conventional planar deposition, facilitating Li nucleation and growth along three-dimensional electronic percolation pathways. This spatially distributed, lateral plating morphology significantly reduced charge-transfer resistance, suppressed dendrite formation, and mitigated cell degradation under high charging currents. Consequently, the ASEI-enabled Li metal electrode maintained low overpotentials at an areal capacity of 10&#xa0;mAh&#xa0;cm<sup>−2</sup> and a current density of 20&#xa0;mA&#xa0;cm<sup>−2</sup> for over 300 h, while demonstrating outstanding rate capability and long-term cyclability in LiFePO<sub>4</sub>(LFP)‖Li and LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811)‖Li full cells. By elucidating these intrinsic anode behaviors, our findings establish a fundamental design strategy for high-rate performance, potentially advancing the commercialization of Li metal batteries. <MediaObject ID="MO685"> <ImageObject Color="Color" FileRef="MediaObjects/40820_2026_2146_Figa_HTML.png" Format="PNG" Height="719" Rendition="HTML" Resolution="300" Type="LinedrawHalftone" Width="968" /> </MediaObject></p>

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Expediting Lithium Electrochemistry via a Bilayer for High-Rate Lithium Metal Batteries

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年3月19日

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  • Dongjoo Park,
  • Dong-Wan Kim

摘要

The intrinsic characteristics of the Li metal anode, particularly its ultra-high specific capacity (3860 mAh g−1) and low redox potential (−3.04 V vs. SHE), theoretically make it ideal for high-rate charge/discharge operations. However, the high Li self-diffusion barrier causes uncontrolled plating/stripping dynamics and severe volume fluctuations, hindering stable performance at elevated current densities. In this study, we introduced an artificial solid-electrolyte interphase (ASEI) engineered with a bilayer that transcends conventional planar deposition, facilitating Li nucleation and growth along three-dimensional electronic percolation pathways. This spatially distributed, lateral plating morphology significantly reduced charge-transfer resistance, suppressed dendrite formation, and mitigated cell degradation under high charging currents. Consequently, the ASEI-enabled Li metal electrode maintained low overpotentials at an areal capacity of 10 mAh cm−2 and a current density of 20 mA cm−2 for over 300 h, while demonstrating outstanding rate capability and long-term cyclability in LiFePO4(LFP)‖Li and LiNi0.8Co0.1Mn0.1O2 (NCM811)‖Li full cells. By elucidating these intrinsic anode behaviors, our findings establish a fundamental design strategy for high-rate performance, potentially advancing the commercialization of Li metal batteries.