Alumina - Stabilized SEI and CEI in Potassium Metal Batteries.

Aluminum oxide (Al2O3) nanopowder is spin-coated onto both sides of commercial polypropene separator to create artificial solid-electrolyte interphase (SEI) and artificial cathode electrolyte interface (CEI) in potassium metal batteries (KMBs). This significantly enhances the stability, including of KMBs with Prussian Blue (PB) cathodes. For example, symmetric cells are stable after 1,000 cycles at 0.5 mA/cm2-0.5 mAh/cm2 and 3.0 mA/cm2-0.5 mAh/cm2. Alumina modified separators promote electrolyte wetting and increase ionic conductivity (0.59 vs. 0.2 mS/cm) and transference number (0.81 vs. 0.23). Cryo-stage focused ion beam (cryo-FIB) analysis of cycled modified anode demonstrates dense and planar electrodeposits, versus unmodified baseline consisting of metal filaments (dendrites) interspersed with pores and SEI. Alumina-modified CEI also suppresses elemental Fe crossover and reduces cathode cracking. Mesoscale modeling of metal - SEI interactions captures crucial role of intrinsic heterogeneities, illustrating how artificial SEI affects reaction current distribution, conductivity and morphological stability.

Heterogeneous Solid Electrolyte Interphase Interactions Dictate Interface Instability in Sodium Metal Electrodes.

Sodium (Na) metal batteries have attracted recent attention due to their low cost and high abundance of Na. However, the advancement of Na metal batteries is impeded due to key challenges such as dendrite growth, solid electrolyte interphase (SEI) fracture, and low Coulombic efficiency. This study examines the coupled electro-chemo-mechanical interactions governing the electrodeposition stability and morphological evolution at the Na/electrolyte interface. The SEI heterogeneities influence transport and reaction kinetics leading to the formation of current and stress hotspots during Na plating. Further, it is demonstrated that the heterogeneity-induced Na metal evolution and its influence on the stress distribution critically affect the mechanical overpotential, contributing to a faster SEI failure. The analysis reveals three distinct failure mechanisms-mechanical, transport, and kinetic-that govern the onset of instabilities at the interface. Finally, a comprehensive comparative study of SEI failure in Na and lithium (Li) metal anodes illustrates that the electrochemical and mechanical characteristics of the SEI are crucial in tailoring the anode morphology and interface stability. This work delineates mechanistic stability regimes cognizant of the SEI attributes and underlying failure modes and offers important guidelines for the design of artificial SEI layers for stable Na metal electrodes.

Synergistic Evolution of Alloy Nanoparticles and Carbon in Solid-State Lithium Metal Anode Composites at Low Stack Pressure.

Solid-state batteries with Li metal anodes can offer increased energy density compared to Li-ion batteries. However, the performance of pure Li anodes has been limited by morphological instabilities at the interface between Li and the solid-state electrolyte (SSE). Composites of Li metal with other materials such as carbon and Li alloys have exhibited improved cycling stability, but the mechanisms associated with this enhanced performance are not clear, especially at the low stack pressures needed for practical viability. Here, we investigate the structural evolution and correlated electrochemical behavior of Li metal composites containing reduced graphene oxide (rGO) and Li-Ag alloy particles. The nanoscale carbon scaffold maintains homogeneous contact with the SSE during stripping and facilitates Li transport to the interface; these effects largely prevent interfacial disconnection even at low stack pressure. The Li-Ag is needed to ensure cyclic refilling of the rGO scaffold with Li during plating, and the solid-solution character of Li-Ag improves cycling stability compared to other materials that form intermetallic compounds. Full cells with sulfur cathodes were tested at relatively low stack pressure, achieving 100 stable cycles with 79% capacity retention.