Low‐Temperature High‐Rate Capabilities of Lithium Batteries via Polarization‐Assisted Ion Pathways

Abstract

On‐board vehicle applications dictate the need for improved low‐temperature power densities of rechargeable batteries. Integration of high‐permittivity artificial dielectric solid electrolyte interfaces (SEIs) into the lithium ion battery architecture is a promising path to satisfy this need. The relationship between the permittivity of various artificial dielectric SEIs and the resulting high‐rate capability at low temperatures is investigated. Room‐temperature studies reveal a weak relationship between these variables. However, at low temperatures, the correlation between the larger permittivity of the dielectric SEIs and the greater high‐rate capabilities of the cells is striking. The high‐rate capabilities for pulsed laser deposition‐synthesized cathode thin films with various BaTiO3 (BTO) SEIs covering configurations are evaluated. A remarkable improvement in the high‐rate capability is observed for LiCoO2 (LCO) modified with dot BTOs, while the rate capability for planar BTO (fully covered LCO) is weakened significantly. A series of experimental results prove that a large polarization, P, in the dielectric SEIs intensified with permittivity accelerates interfacial charge transfer near the dielectrics–LCO–electrolyte triple junction.

In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries

“…According to the Lorentz hypothesis, the built-in electric field intensity of CNs (E in ) is directly proportional to the electric field intensity E SCL of the SCL and the dielectric constant of the CNs (ε CNs ). The SCL is caused by the chemical potential difference between the electrolyte and cathode (ϕ electrolyte −ϕ cathode ), and the dielectric constants of CNs strongly depend on their particle sizes (d CNs ) 57,58 . Furthermore, the redistribution of lithium ions at the TPI is also determined by E in and the distance L between neighboring BTO nanoparticles.…”

Pulsed Laser Deposition‐based Thin Film Microbatteries

“…[33] Interesting recent work has termed certain coating materials as artificial solid electrolyte interface layers (SEI), whereby the coverage of dielectric BaTiO 3 on LiCoO 2 is investigated revealing the benefits of partial or full coverage in various facets of cell performance. [34] The intention of such work is to pre-generate a portion of the SEI that often forms during initial cycling of a lithium-ion battery.…”

Ultrafast Ion Transport via Dielectric Nanocube Interface

“…[ 8–15 ] A great advance occurred with the incorporation of the BaTiO 3 (BTO)‐based “artificial dielectric interfaces” architecture into the active materials–electrolyte interface. [ 16–19 ] This strategy has led to a significant reduction in the R ct of LIBs, which in turn has yielded extremely high rate capabilities despite the incorporation of insulators traditionally used in ceramic capacitors. [ 20–22 ] Our previous research identified the fast Li‐ion pathway via a dielectric interface using theoretical and experimental approaches.…”