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

Tian, Mengyu; Qiao, Ronghan; Cen, Guanjun; Tian, Li; Ben, Liubin; Yu, Hailong; De Volder, Michael; Zhao, Chenglong et al. · Nat Commun · 2025

basic_science · Level V

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Abstract

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.