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In this Nature Paper, we introduce a grain-boundary modification strategy for garnet solid electrolytes by forming amorphous zirconia at grain boundaries during sintering, producing a two-phase microstructure with reduced porosity. This engineered electrolyte suppresses lithium dendrite propagation, boosts critical current density, and leads to improved cycling stability compared to conventional single-phase garnets, offering a promising route for safer lithium metal solid-state batteries.
The article "Understanding the Role of Borohydride Doping in Electrochemical Stability of Argyrodite Li6PS5Cl Solid-State Electrolyte", demonstrates how lithium borohydride (LiBH₄) doping enhances the electrochemical stability of argyrodite Li₆PS₅Cl solid-state electrolyte (LBH-LPSCl) by forming a tri-layer solid electrolyte interphase (SEI) that blocks electrons yet facilitates Li⁺ transport at interfaces. SSEs with 5 wt% BH₄ exhibit much higher critical current densities and stable cycling in both symmetric Li cells and anode-free full cells, with reduced interfacial resistance and improved room-temperature performance.
This work presents a reactive carbide-based synthesis of NASICON-type sodium solid-state electrolyte (Na₁₊ₓZr₂SiₓP₃₋ₓO₁₂) that uses the exothermic reaction of carbide precursors to yield highly dense ceramics with controlled secondary phases, in sharp contrast to conventional oxide routes. The resulting carbide-derived NZSP shows improved dendrite suppression and higher critical current densities in sodium metal symmetric cells due to optimized microstructure. Small, disperse zirconia toughen the electrolyte, while brittle glasses typically found in the oxide-route are present but non-percolated in the carbide NZSP.
In the article "Control of Two Solid Electrolyte Interphases at the Negative Electrode of an Anode-Free All Solid-State Battery based on Argyrodite Electrolyte", we identify the three critical interfaces in anode-free all-solid-state batteries (AF-ASSBs) — the lithium metal–solid electrolyte interphase (SEI-1), the lithium–current collector interface, and the collector–solid electrolyte interphase (SEI-2) — and demonstrates that controlling them with a 140 nm Mg/30 nm W bilayer on Cu suppresses detrimental interfacial reactions in argyrodite Li₆PS₅Cl solid electrolytes. The engineered bilayer enables state-of-the-art performance in both half-cells and full NMC811 cells, delivering >150 cycles with Coulombic efficiency >99.8 % and 86.5 % capacity retention at high cathode loading, by stabilizing SEI formation, promoting conformal Li wetting, and preventing ongoing SEI-2 growth that drives degradation.
This Advanced Materials article shows that the microstructure of argyrodite Li₆PS₅Cl solid electrolyte critically influences lithium metal electrodeposition and dissolution, and that planetary milling in wet m-xylene progressively refines grains and pores, increases density, and smoothens the Li|SSE interface. These microstructural changes reduce local hardness variations, promote uniform early-stage electrodeposition on foil collectors, and stabilize the solid electrolyte interphase, and, for the first time, directly identify short-circuiting Li dendrites intergranularly filling interparticle voids; mesoscale modeling links interface morphology to electrochemical instability via heterogeneous reaction current distribution.
In this investigation of garnet solid-state electrolytes (specifically Ta-doped Li₆.₄La₃Zr₁.₄Ta₀.₆O₁₂), samples prepared with high-energy milling achieve significantly higher density, reduced grain size, and lower surface roughness at the Li contact than conventionally sintered compacts. These optimized microstructural features enable symmetric cells to cycle at constant capacity with greatly enhanced critical current density (1.4 vs. 0.3 mA cm⁻²), reveal that lithium dendrites propagate preferentially through regions of small grains and pores, and show that both grain size distribution and internal porosity crucially affect electrical short-circuit failure — with modeling highlighting the interplay between reaction and stress heterogeneities that focus current and promote plating at grain boundaries.
This paper reports that a thin intermetallic Li₂Te–LiTe₃ bilayer formed from 2D tellurene effectively stabilizes the solid electrolyte interphase between lithium metal and Li₆PS₅Cl argyrodite solid electrolyte. When applied via mechanical rolling or direct transfer, the bilayer impedes electrolyte decomposition, enabling symmetric cells to run 300 cycles (1800 h) at practical current densities while cryo-FIB and Raman mapping show that the engineered SEI dramatically suppresses deep solid electrolyte reduction that otherwise leads to voiding in both lithium and electrolyte; DFT and mesoscale modeling further elucidate interfacial thermodynamic and stress effects linked to heterogeneous reaction fronts.
In this article-Stable Anode-Free All-Solid-State Lithium Battery through Tuned Metal Wetting on the Copper Current Collector - we introduced a lithiophilic Li₂Te coating on copper current collectors for anode-free all-solid-state batteries with Li₆PS₅Cl solid electrolyte, this study demonstrates substantial improvements in lithium nucleation and growth behavior. The Li₂Te layer dramatically lowers electrodeposition and electrodissolution overpotentials, enhances Coulombic efficiency (with AF-ASSBs achieving >99 % cycling efficiency and uniform >70 µm lithium deposition), and yields uniform, dendrite-free metal microstructure at the collector–electrolyte interface, whereas unmodified Cu produces inhomogeneous deposits, dead metal, and thick, porous SEI; DFT and mesoscale models provide insight into the favorable nucleation and growth dynamics mediated by Li₂Te.
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