Sulfur defect engineering controls Li<sub>2</sub>S crystal orientation towards dendrite-free lithium metal batteries.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 40169624.
- Also identified by DOI 10.1038/s41467-025-57572-5 and PMC identifier 11962132.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
Abstract
Controlling nucleation and growth of Li is crucial to avoid dendrite formation for practical applications of lithium metal batteries. Li<sub>2</sub>S has been exemplified to promote Li transport, but its crystal orientation significantly influences the Li deposition behaviors. Here, we investigate the interactions between Li and various surface structures of Li<sub>2</sub>S, and reveal that the Li<sub>2</sub>S(111) plane exhibits the highest Li affinity and the lowest diffusion barrier, leading to dense Li deposition. Using sulfur defect engineering for Li<sub>2</sub>S crystal orientation control, we construct three-dimensional vertically oriented Li<sub>2</sub>S(111)@Cu nanorod arrays as a Li metal electrode substrate and identify a substrate-dependent Li nucleation process and a facet-dependent growth mode. Furthermore, we demonstrate the versatility of the Li<sub>2</sub>S(111)@Cu substrate when paired with two positive electrodes: achieving an initial discharge capacity of 138.8 mAh g<sup>-1</sup> with 88% capacity retention after 400 cycles at 83.5 mA g<sup>-1</sup> with LiFePO<sub>4</sub>, and an initial discharge capacity of 181 mAh g<sup>-1</sup> with 80% capacity retention after 160 cycles at 60 mA g<sup>-1</sup> with commercial LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> positive electrode (4 mAh cm<sup>-2</sup>).