Lithiophilic Interlayer with Electrolyte-Reservoir and Dendrite-Buffer for High-Performance Lithium Metal Batteries

Uneven local electric fields and limited nucleation sites at the reaction interface can lead to the formation of hazardous lithium (Li) dendrites, posing a significant safety risk and impeding the practical utilization of Li metal anodes (LMAs). Here, we present a method utilizing atomic layer deposition (ALD) to create lithiophilic titanium nitride (TiN) sites on carbon nanotubes (CNTs) surfaces, integrated with nanocellulose to form a lithiophilic interlayer (NFCP@TN). This interlayer, which is highly flexible and electrolyte-wettable, functions as a current collector and host material for LMAs. The uniform deposition of Li is facilitated by the synergistic interplay of the lithiophilic active sites TiN, the conductive CNT network, and excellent electrolyte wettability of nanocellulose. As a result, Li preferentially adsorbs on TiN sheaths with lower diffusion barriers, leading to controlled nucleation sites and dendrite-free Li deposition. Furthermore, the well-designed NFCP@TN interlayer exhibits exceptional electrochemical performance and significantly extended cycle life when paired LMA with high areal capacity NCM811 (5.0 mAh cm^-2) electrodes.