<p>Pairing high-energy nickel-rich cathodes with current collectors as anodes presents a compelling strategy to significantly boost the specific energy of rechargeable lithium-ion batteries, driving progress toward a transportation revolution. However, the limited active lithium inventory sourced by the cathodes tend to be rapidly consumed by irreversible Li plating/stripping and interfacial side reactions. To address these limitations, we propose a dual-gradient metal layer as an innovative solution to mitigate active Li loss by promoting uniform Li deposition and in situ formation of a stable solid electrolyte interphase. The operation of these batteries is investigated using a combination of electrochemical and chemical techniques to differentiate dead Li and interphase-bound Li inventory loss as well as material characterization methods to analyse the plated Li and interfacial composition and morphology. The developed dual gradient metal layer-based 600 mAh LiNi<sub>0.9</sub>Co<sub>0.05</sub>Mn<sub>0.05</sub>O<sub>2</sub> | |Cu pouch cells achieve an areal capacity of 7.25 mAh cm<sup>−2</sup> and deliver an 80% capacity retention over 160 cycles. We show that the proposed approach is compatible with a range of different metal materials, offering a promising path toward next generation long-lasting, high-energy, initially active material-free anode based Li metal batteries.</p>

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Dual-gradient metal layer for practicalizing high-energy lithium batteries

  • Mengyu Tian,
  • Ronghan Qiao,
  • Guanjun Cen,
  • Li Tian,
  • Liubin Ben,
  • Hailong Yu,
  • Michael De Volder,
  • Chenglong Zhao,
  • Qidi Wang,
  • Xuejie Huang

摘要

Pairing high-energy nickel-rich cathodes with current collectors as anodes presents a compelling strategy to significantly boost the specific energy of rechargeable lithium-ion batteries, driving progress toward a transportation revolution. However, the limited active lithium inventory sourced by the cathodes tend to be rapidly consumed by irreversible Li plating/stripping and interfacial side reactions. To address these limitations, we propose a dual-gradient metal layer as an innovative solution to mitigate active Li loss by promoting uniform Li deposition and in situ formation of a stable solid electrolyte interphase. The operation of these batteries is investigated using a combination of electrochemical and chemical techniques to differentiate dead Li and interphase-bound Li inventory loss as well as material characterization methods to analyse the plated Li and interfacial composition and morphology. The developed dual gradient metal layer-based 600 mAh LiNi0.9Co0.05Mn0.05O2 | |Cu pouch cells achieve an areal capacity of 7.25 mAh cm−2 and deliver an 80% capacity retention over 160 cycles. We show that the proposed approach is compatible with a range of different metal materials, offering a promising path toward next generation long-lasting, high-energy, initially active material-free anode based Li metal batteries.