<p>The development of lithium metal batteries (LMBs) face numerous challenges, particularly in terms of safety, cycling stability, electrochemical reversibility, and cost control, which are largely associated with Li dendrite formation. In this study, three-dimensional hierarchical porous copper (3DBO-Cu) current collectors (CCs) were fabricated from commercial brass foils using a gradient vapor phase dealloying (VPD) method under an oxygen-free atmosphere in a tube furnace at atmospheric pressure. 3DBO-Cu contains abundant hierarchical macropores with sizes ranging from 1 to 10&#xa0;µm and 200 to 500&#xa0;nm. A lithiophilic Li-Cu alloy (LiCu<sub>x</sub>) layer formed spontaneously on the porous framework through a high-temperature Li melting method, preserving the 3D morphology and facilitating rapid infusion of molten Li across the entire surface. Furthermore, the 3DBO-Cu exhibited a much lower initial nucleation overpotential (20&#xa0;mV) compared to planar Cu foil (91&#xa0;mV). This revealed that the synergistic effect of the porous structure and trace residual Zn on the surface significantly reduced the nucleation barrier of Li on Cu CCs. When paired with an LiFeO<sub>4</sub> (LFP) cathode, the full cell (LFP||Li/3DBO-Cu) demonstrated an initial specific capacity of 148.08 mAh·g<sup>−1</sup> and maintained a discharge capacity of 132.27 mAh·g<sup>−1</sup> with 89.32% capacity retention after 900 cycles at 1C, along with high and stable coulombic efficiency (CE).</p>

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Preparation of three-dimensional hierarchical porous copper current collectors via gradient vapor phase dealloying for stable lithium metal anode

  • Yong Li,
  • Siqi Xiao,
  • Shuzhen Liang,
  • Yufeng Liu,
  • Jiahao Hu,
  • Ruyu Wu,
  • Chengyu Zhang

摘要

The development of lithium metal batteries (LMBs) face numerous challenges, particularly in terms of safety, cycling stability, electrochemical reversibility, and cost control, which are largely associated with Li dendrite formation. In this study, three-dimensional hierarchical porous copper (3DBO-Cu) current collectors (CCs) were fabricated from commercial brass foils using a gradient vapor phase dealloying (VPD) method under an oxygen-free atmosphere in a tube furnace at atmospheric pressure. 3DBO-Cu contains abundant hierarchical macropores with sizes ranging from 1 to 10 µm and 200 to 500 nm. A lithiophilic Li-Cu alloy (LiCux) layer formed spontaneously on the porous framework through a high-temperature Li melting method, preserving the 3D morphology and facilitating rapid infusion of molten Li across the entire surface. Furthermore, the 3DBO-Cu exhibited a much lower initial nucleation overpotential (20 mV) compared to planar Cu foil (91 mV). This revealed that the synergistic effect of the porous structure and trace residual Zn on the surface significantly reduced the nucleation barrier of Li on Cu CCs. When paired with an LiFeO4 (LFP) cathode, the full cell (LFP||Li/3DBO-Cu) demonstrated an initial specific capacity of 148.08 mAh·g−1 and maintained a discharge capacity of 132.27 mAh·g−1 with 89.32% capacity retention after 900 cycles at 1C, along with high and stable coulombic efficiency (CE).