Shi Jie, Koketsu Toshinari, Zhu Zhenglu, Yang Menghao, Sui Lijun, Liu Jie, Tang Mingxue, Deng Zhe, Liao Mengyi, Xiang Jingwei, Shen Yue, Qie Long, Huang Yunhui, Strasser Peter, Ma Jiwei
Shanghai Key Laboratory for R&D and Application of Metallic Functional Materials, Institute of New Energy for Vehicles, School of Materials Science and Engineering, Tongji University, Shanghai, China.
Department of Chemistry, Technical University Berlin, Berlin, Germany.
Nat Mater. 2024 Dec;23(12):1686-1694. doi: 10.1038/s41563-024-01997-8. Epub 2024 Sep 2.
'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 Sn at the initial charging process builds a stable lithophilic layer of CuSn 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.
“无阳极”锂金属电池具有尽可能高的能量密度，但在碳酸盐电解质中运行时面临低锂库仑效率的问题。在此，我们报告了在碳酸盐电解质中使用p区辛酸亚锡添加剂提高无阳极锂金属电池的性能。我们表明，辛酸部分在铜基底上的优先吸附诱导形成了无碳酸盐的保护层，该保护层抑制了副反应并有助于锂的均匀沉积。同时，在初始充电过程中锡的还原形成了稳定的亲锂性铜锡合金和锡层，提高了锂与铜基底之间的亲和力。值得注意的是，添加辛酸亚锡添加剂的无阳极锂金属软包电池表现出良好的循环稳定性，库仑效率高达约99.1%。此外，这种原位p区层电镀策略也在其他类型的p区金属辛酸盐以及钠金属电池系统中得到了验证，证明了其高度的通用性。
