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In situ p-block protective layer plating in carbonate-based electrolytes enables stable cell cycling in anode-free lithium batteries

  • Jie Shi,
  • Toshinari Koketsu,
  • Zhenglu Zhu,
  • Menghao Yang,
  • Lijun Sui,
  • Jie Liu,
  • Mingxue Tang,
  • Zhe Deng,
  • Mengyi Liao,
  • Jingwei Xiang,
  • Yue Shen,
  • Long Qie,
  • Yunhui Huang,
  • Peter Strasser,
  • Jiwei Ma

摘要

‘Anode-free’ Li metal batteries offer the highest possible energy density but face low Li coulombic efficiency when operated in carbonate electrolytes. Here we report a performance improvement of anode-free Li metal batteries using p-block tin octoate additive in the carbonate electrolyte. We show that the preferential adsorption of the octoate moiety on the Cu substrate induces the construction of a carbonate-less protective layer, which inhibits the side reactions and contributes to the uniform Li plating. In the mean time, the reduction of Sn2+ at the initial charging process builds a stable lithophilic layer of Cu6Sn5 alloy and Sn, improving the affinity between the Li and the Cu substrate. Notably, anode-free Li metal pouch cells with tin octoate additive demonstrate good cycling stability with a high coulombic efficiency of ~99.1%. Furthermore, this in situ p-block layer plating strategy is also demonstrated with other types of p-block metal octoate, as well as a Na metal battery system, demonstrating the high level of universality.