In Situ Formation of Bifunctional Interlayer on 3D Conductive Scaffold
for Dendrite Free Li Metal Batteries
Abstract
Regulating lithium (Li) plating/stripping behavior in three-dimensional
(3D) conductive scaffolds is critical to stabilize Li metal batteries
(LMBs). Surface protrusions and roughness in these scaffolds can induce
uneven distributions of the electric fields and ionic concentrations,
forming ’hot spots’. Hot spots may cause uncontrollable Li dendrites
growth, presenting significant challenges to the cycle stability and
safety of LMBs. To address these issues, we construct a Li ionic
conductive-dielectric gradient bifunctional interlayer (ICDL) onto 3D
Li-injected graphene/carbon nanotube scaffold (LGCF) via in situ
reaction of exfoliated hexagonal boron nitride (fhBN) and molten Li.
Microscopic and spectroscopic analyses reveal that ICDL consists of
fhBN-rich outer layer and inner layer enriched with Li3N and Li-boron
composites (Li-B). The outer layer utilizes dielectric properties to
effectively homogenize the electric field, while the inner layer ensures
high Li ion conductivity. Moreover, DFT calculations indicate that ICDL
can effectively adsorb Li and decrease the Li diffusion barrier,
promoting enhanced Li ion transport. The modulation of Li kinetics by
ICDL increases the critical length of the Li nucleus, enabling
suppression of Li dendrite growth. Attributing to these advantages, the
ICDL coated LGCF (ICDL@LGCF) demonstrates impressive long term cycle
performances in both symmetric cells and full cells.