Lithium Dendrite Suppression with a Silica Nanoparticle-Dispersed Colloidal Electrolyte

Abstract

Developing a safe and long-lasting lithium (Li) metal battery is crucial for high-energy applications. However, its poor cycling stability due to Li dendrite formation and excessive Li pulverization is the major hurdle for its practical applications. Here, we present a silica (SiO2) nanoparticle-dispersed colloidal electrolyte (NDCE) and its design principle for suppressing Li dendrite formation. SiO2 nanoclusters in the NDCE play roles in enhancing the Li+ transference number and increasing the Li+ diffusivity in the vicinity of the Li-plating substrate. The NDCE enables less-dendritic Li plating by manipulating the nucleation-growth mode and extending Sand’s time. Moreover, SiO2 can interplay with the electrolyte components at the Li-metal surface, enriching fluorinated compounds in the solid electrolyte interface layer. The initial control of the Li plating morphology and SEI structure by the NDCE leads to a more uniform and denser Li deposition upon subsequent cycling, resulting in threefold enhancement of the cycle life. The efficacy of the NDCEs has been further demonstrated by the practical battery design, featuring a commercial-level cathode and thin Li-metal (40 μm) anode.

Comprehensive Analyses of Aqueous Zn Metal Batteries: Characterization Methods, Simulations, and Theoretical Calculations

“…On the basis of Sand's time model, reducing the local current density can retard the initial formation of dendrites. [ 127–130 ] Moreover, this 3D VG scaffold could induce a uniform distribution of the electric field at an early stage and be maintained in subsequent cycles (Figure 10e). In contrast, the 2D planar configuration was apt to initiate individual nucleation points and further developed into an uneven electric field (Figure 10f), which would lead to subsequent growth of Zn dendrites.…”

Nonflammable Gel Polymer Electrolyte with Ion-Conductive Polyester Networks for Sodium Metal Cells with Excellent Cycling Stability and Enhanced Safety

“…As presented in Figure b, the suppressed electrolyte decomposition at the Na electrode induces the formation of a thin SEI layer and uniform Na deposition. The large amounts of free Na + ions in the GPE can also extend the Sand’s time (τ) when the Na + ion concentration decreases to zero at the electrolyte/electrode interface, which suppresses Na dendritic growth. , From these results, it can be said that the use of GPE can enhance the reversibility and cyclability of the Na plating/stripping reaction.…”

Complex Growth Behavior of Li Dendrites in Al2O3 Nanoparticles‐Driven Viscoelastic Electrolytes for Lithium Metal Batteries: Dynamic versus Quasistatic Rheology

“…The improved ionic conductivity of viscoelastic electrolytes was known to be due to the faster interfacial conduction pathway of Li + cations through space charge layers on the Al 2 O 3 surface, which is dependent on the acidic nature and the percolative network formation of oxide nanoparticles (Figure S5, Supporting Information). [ 57–59 ] This interfacial behavior also contributed to increasing the transference number (t Li+ ) of Li + cations in viscoelastic electrolytes compared to the Newtonian electrolyte. The transference number of Li + cations were estimated using the Bruce‐Vincent equation [ 65 ] where I 0 , I S , R 0 , R S , and ∆ V stand for initial and steady state currents, initial and steady state resistances, and polarization potential, respectively.…”

“…[ 21–28 ] Various three‐dimensional host structures have also been suggested to reduce volume change during cycling. [ 29–35 ] In addition, high salt concentration electrolytes, [ 36–39 ] electrolyte additives, [ 40–42 ] single ion conducting membranes, [ 43–47 ] and viscoelastic electrolytes [ 48–62 ] have been introduced to homogenize Li + ion flux.…”