Solid interface electrochemistry between LiCoO<sub>2</sub> and solid-state electrolytes.
basic_science · Level V
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- Record sourced from PubMed, PMID 42600013.
- Also identified by DOI 10.1126/sciadv.aef1533.
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Abstract
Strategies to optimize the cathode/solid electrolyte interphase (CSEI) have been developed to improve the high voltage durability of LiCoO<sub>2</sub> (LCO), yet the underlying interfacial mechanism remains unclear. Here, we construct a stable oxyhalide-derived CSEI for all-solid-state batteries (ASSBs) to identify the key interfacial features required for high-voltage operation. At 4.6 volts, commercial LCO coupled with Li<sub>6</sub>PS<sub>5</sub>Cl (LPSC) suffers from severe interfacial instability, sluggish Li<sup>+</sup> transport, and continuous side reactions. By introducing LiNbOCl<sub>4</sub> (LNOC), an in situ formed CSEI rich in Li-Cl/Nb-O/Nb-O-Cl species is established, lowering the interfacial energy barrier to 0.363 electron volts and enhancing interfacial toughness and ionic conductivity. This stabilized interface suppresses lattice oxygen activity, accelerates Li<sup>+</sup> transport, and improves the reversibility of O3/H1-3 phase transitions. Consequently, LCO|LNOC|LPSC|Li-In ASSBs deliver 95.8% capacity retention after 500 cycles at ∼1.0 C-rate with an LCO loading of 15.31 milligrams per square centimeter. The pouch cell achieves 90% initial Coulombic efficiency and stable cycling over 50 cycles.