Laser‐Structured Graphite Paper Hybrid Anode with Selective Lithiophilic Grooves for Controlled Lithium Metal Deposition

Abstract Lithium (Li) metal anodes offer significantly higher theoretical capacity than graphite anodes but face challenges in terms of stability and safety due to dendrite growth and solid electrolyte interphase (SEI) instability. To address these issues, a hybrid Li‐ion/metal anode is proposed to enhance cycling stability by selectively forming lithiated graphite, thereby promoting uniform Li deposition. By laser‐processing commercial graphite paper (GP), a laser‐ablated graphite paper (LGP) anode featuring grooved structures enriched with oxygen‐containing functional groups is fabricated. These structures expose electrochemically active edge planes that facilitate Li‐ion adsorption and intercalation in graphite flakes. The lithophilic functional groups and lithiated graphite (LiC6) inside grooves promote selective Li metal deposition, inhibit dendrite growth, and enhance energy density. The Li||LGP half‐cell operated stably over 300 cycles at 1 mA cm−2 with a Coulombic efficiency over 99%. LGP||LiFePO4 full‐cell maintained a capacity of 157 mAh g−1 after 150 cycles at 0.5 C, compared to 137.5 mAh g−1 for GP||LiFePO4 cells. The LGP full‐cell also shows a capacity of 104 mAh g−1 with 91% capacity retention after 500 cycles at 5 C, whereas the GP full‐cell declined rapidly. These results highlight the potential of the approach for improving the cycling stability and performance of Li metal batteries.