<p>The practical application of lithium metal batteries is hindered by the heterogeneous solid-electrolyte interphase (SEI), which undergoes repeated cracking and reconstruction during cycling, thereby exacerbating lithium dendrite growth. To address this issue, we propose an in-situ reconstruction strategy for the SEI layer by introducing the functional additive 1,3,5-trioxane (TO), which helps to homogenize lithium transport and enhance mechanical stability. By participating in the Li<sup>+</sup> solvation structure, TO facilitates the formation of a homogeneous and mechanically robust SEI, which preferentially promotes the formation of a polyoxymethylene (POM) phase and enriches LiF content within the SEI. This tailored interface significantly improves the uniformity of lithium deposition and interfacial compatibility. In coin cells employing a high-loading LiNi<sub>0.90</sub>Co<sub>0.05</sub>Mn<sub>0.05</sub>O<sub>2</sub> cathode (7.37&#xa0;mg cm<sup>− 2</sup>) and an ultrathin lithium anode (50&#xa0;μm), the TO-modified electrolyte enables a capacity retention of 73.1% after 200 cycles at 0.5&#xa0;C, substantially outperforming the conventional electrolyte that retained only 25.9%. These results demonstrate the promising potential of this electrolyte design for high-energy-density lithium metal batteries.</p>

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Significantly improved capacity retention of lithium metal batteries enabled by a 1,3,5-Trioxane electrolyte additive

  • Jing Wang,
  • Chuan Yao,
  • Chang Su

摘要

The practical application of lithium metal batteries is hindered by the heterogeneous solid-electrolyte interphase (SEI), which undergoes repeated cracking and reconstruction during cycling, thereby exacerbating lithium dendrite growth. To address this issue, we propose an in-situ reconstruction strategy for the SEI layer by introducing the functional additive 1,3,5-trioxane (TO), which helps to homogenize lithium transport and enhance mechanical stability. By participating in the Li+ solvation structure, TO facilitates the formation of a homogeneous and mechanically robust SEI, which preferentially promotes the formation of a polyoxymethylene (POM) phase and enriches LiF content within the SEI. This tailored interface significantly improves the uniformity of lithium deposition and interfacial compatibility. In coin cells employing a high-loading LiNi0.90Co0.05Mn0.05O2 cathode (7.37 mg cm− 2) and an ultrathin lithium anode (50 μm), the TO-modified electrolyte enables a capacity retention of 73.1% after 200 cycles at 0.5 C, substantially outperforming the conventional electrolyte that retained only 25.9%. These results demonstrate the promising potential of this electrolyte design for high-energy-density lithium metal batteries.