In Situ Formation of an Artificial Lithium Oxalate-Rich Solid Electrolyte Interphase on 3D Ni Host for Highly Stable Lithium Metal Batteries.

Abstract

Li metal, with a high theoretical capacity, is considered the most promising anode for next-generation high-energy-density batteries. However, the commercialization of the Li metal anode is limited owing to its high reactivity, significant volume expansion, continuous solid electrolyte interphase (SEI) layer degradation caused by undesirable Li deposition, and uncontrollable dendrite growth. This study demonstrates the in situ construction of a Li2C2O4-enriched SEI layer from NiC2O4 nanowires on three-dimensional Ni foam. The lithiophilic Li2C2O4-enriched SEI layer provides a uniform distribution of the electrical field and sufficient nucleation and deposition sites for Li without dendrite formation. Consequently, the stable Li2C2O4-enriched SEI layer successfully inhibits the formation of lithium dendrites, resulting in reversible Li stripping/plating behavior, maintained over an extended period of 5000 h with a deposition capacity of 1 mAh cm-2 at 1 mA cm-2. Additionally, a high cycling stability is observed in the full cell test with ∼70% capacity retention after 1300 cycles at 3 C. This approach offers a large-scale and facile synthesis process via the in situ precipitation growth of NiC2O4 followed by lithiation to form Li2C2O4. Furthermore, the significant stability of the Li2C2O4-enriched SEI layer aids the design of in situ-constructed SEI layers for highly stable Li metal batteries.