An ultrathick lithium metal anode (LMA) is a prerequisite for developing practical lithium–sulfur (Li–S) batteries that simultaneously meet the requirements of high areal capacity, lean electrolyte, and limited excess Li. Inspired by the electrochemical process for an organosulfur cathode, herein, we reconfigure such a sulfur cathode by using an overlithiation strategy to enable the formation of a high performance LMA. Specifically, an applicable ultrathick LMA is successfully constructed by overlithiating a well-known organosulfur cathode material, sulfurized polyacrylonitrile (SPAN). SPAN contains a polymeric pyridine structure with an outstanding lithium-ion affinity, so that it can act as a lithiophilic matrix. More importantly, a Li₂S-rich solid electrolyte interphase (SEI) can be generated on the surface of SPAN during the overlithiation process. The synergistic effect of the lithiophilic matrix and a robust SEI leads to a dense deposition of lithium, which enables one to form an ultrathick LMA (159 μm, 30 mAh cm^–2) with high Coulombic efficiency (99.7%). Such an LMA paired with a sulfur cathode of high areal capacity (up to 16 mAh cm^–2) shows stable cycling under practical conditions of a lean electrolyte (2.2 μL mg_S^–1) and a negative-to-positive capacity (N/P) ratio as low as 1.3. The applicability of the ultrathick LMA was further verified with Li–S pouch cells, indicating a highly prospective route toward realization of practical Li–S batteries.

中文翻译：

---

通过过度锂化来重新配置有机硫阴极，以使超厚锂金属阳极朝实用锂硫电池的方向发展。

超厚锂金属阳极（LMA）是开发实用的锂硫（Li–S）电池的先决条件，该锂硫电池同时满足高面容量，稀薄电解质和有限的过量Li的要求。受有机硫阴极电化学过程的启发，在本文中，我们通过使用过度锂化策略重新配置了此类硫阴极，以实现高性能LMA的形成。具体而言，通过对已知的有机硫阴极材料硫化聚丙烯腈（SPAN）进行超锂化，成功构建了适用的超厚LMA。SPAN包含具有出色的锂离子亲和力的聚合吡啶结构，因此它可以充当亲硫基质。更重要的是，李₂在过锂化过程中，会在SPAN的表面上生成富含S的固体电解质中间相（SEI）。亲锂基体和强大的SEI的协同作用导致锂的致密沉积，使锂能够形成具有库仑效率（99.7％）的超厚LMA（159μm，30 mAh cm ^–2）。这种LMA与高面积容量（高达16 mAh cm ^–2）的硫阴极配对，在稀薄电解质（2.2μLmg _S ^–1）和负-正容量（N / P）比率低至1.3。Li-S袋式电池进一步验证了超厚LMA的适用性，这表明朝着实现实际Li-S电池的方向发展的可能性很高。