Self-Healing Nucleation Seeds Induced Long-Term Dendrite-Free Lithium Metal Anode

Abstract

Seeded lithium (Li) nucleation has been considered as a promising strategy to achieve uniform Li deposition. However, problems of agglomeration and pulverization quickly invalidate the nucleation seeds, resulting in Li dendrite growth during repeated charge/discharge processes. Herein, liquid gallium−indium (GaIn) nanoparticles with structural self-healing properties are utilized to guide uniform metallic Li nucleation and deposition. Ultrafine GaIn nanoparticles (∼25 nm) uniformly decorated on the surface of carbon layers effectively homogenize the lithium-ion flux. After fully Li stripping, lithiophilic GaIn nanoparticles return to the liquid binary eutectic phase, thereby healing the deformed structure and enabling them to continuously guide dendrite-free Li deposition. Li metal anodes with such nucleation seeds exhibit nearly zero nucleation overpotential even after hundreds of cycles and a high average Coulombic efficiency of 99.03% for more than 400 cycles. The design of self-healing nucleation seeds provides important insights for obtaining high-performance lithium metal anodes.

Synergizing Conformal Lithiophilic Granule and Dealloyed Porous Skeleton toward Pragmatic Li Metal Anodes

“…CE performance was first examined in the half-cell configuration assembled by pairing the routine Li metal with D-Cu@CuSe, while B-Cu-and D-Cu-based half cells were also constructed for comparison. [37][38][39] It is interesting to note that an apparent discharge platform can be observed at %0.8 V (vs. Li/Li þ ) during the initial electrochemical activation process (Figure S9, Supporting Information). Correspondingly, the characteristic peaks assigned to Li 2 Se in the XRD pattern further verify the in situ generation of the Li 2 Se protective layer (Figure S10, Supporting Information).…”

Vertically Aligned MXene Nanosheet Arrays for High‐Rate Lithium Metal Anodes

“…Moreover, the activation energies of lithium‐ion (Li + ) transport through SEI ( E a , SEI ) and charge transfer ( E a , ct ) for v‐Ti 3 C 2 T x electrodes and h‐Ti 3 C 2 T x electrodes were calculated based on Arrhenius law. [ 45,46 ] As shown in Figure 2h, the E a , SEI of v‐Ti 3 C 2 T x (35.27 kJ mol −1 ) was significantly lower than that of h‐Ti 3 C 2 T x electrodes (49.52 kJ mol −1 ). This was because the uniform SEI layer on v‐Ti 3 C 2 T x electrodes could effectively inhibit the accumulation of electrolyte and the formation of a thick solvent‐derived SEI layer, which would significantly block the Li + transportation and increase the activation energy.…”

Anode‐Free Solid‐State Lithium Batteries: A Review

“…proposed the concept of self‐healing nucleation seeds. [ 112 ] The researchers effectively homogenized the lithium‐ion flux by using superfine GaIn nanoparticles (25 nm) uniformly decorated on the surface of the carbon layer. Since the GaIn nanoparticles are uniformly dispersed, the lithiophilic GaIn nanoparticles revert to a liquid binary eutectic phase after complete delithiation, thereby repairing the deformed structure and enabling continuous dendritic‐free lithium deposition.…”