The epitaxial deposition of solid sulfides prefers lateral deposition driven by the superior charge transfer of the conductive substrate to produce a continuous insulating 2D film. This situation not only disables the adsorbing host from controlling the dissolved PSs, but also terminates electrochemical redox when the mass transport and electron transfer are completely blocked by the non-conductive layer. Here, we present that single-atom Co is of significance to control the epitaxial deposition of solid sulfides to promote spherical cumulative deposition with 3D morphology. On the carbon paper (CP), the deposition shows the lateral deposition mode with a much lower capacity. On the single-atom Co decorated carbon paper (CoSAs-CP), it shows the spherical cumulative deposition mode with a high capacity reaching up to its theoretical value. The experimental studies and theoretical calculations reveal that single-atom Co can reconstruct the electronic structure of solid intermediates owing to the d–p hybridization associated with an electron feedback coupling mechanism, which benefits the non-locality of electrons and octahedron–tetrahedron fields of solid intermediates, promoting both the electron transfer and Li transport of longitudinal deposition to balance the lateral deposition so as to sustain the spherical epitaxial deposition.

中文翻译：

---

促进用于大容量Li–S电池的固态硫化物的球形外延沉积

固体硫化物的外延沉积优选由导电基底的优异电荷转移驱动的横向沉积，以产生连续的绝缘2D膜。这种情况不仅使吸附主体无法控制溶解的PS，而且在质量传输和电子转移被非导电层完全阻止时，终止了电化学氧化还原。在这里，我们提出单原子Co对于控制固体硫化物的外延沉积以促进具有3D形态的球形累积沉积具有重要意义。在复写纸（CP）上，沉积显示出横向沉积模式，容量低得多。在单原子的带Co装饰碳纸（CoSAs-CP）上，它显示了球形累积沉积模式，具有高达其理论值的高容量。