The long-standing issue of lithium dendrite growth during repeated deposition or dissolution processes hinders the practical use of lithium-metal anodes for high-energy density batteries. Here, we demonstrate a promising lithiophilic–lithiophobic gradient interfacial layer strategy in which the bottom lithiophilic zinc oxide/carbon nanotube sublayer tightly anchors the whole layer onto the lithium foil, facilitating the formation of a stable solid electrolyte interphase, and prevents the formation of an intermediate mossy lithium corrosion layer. Together with the top lithiophobic carbon nanotube sublayer, this gradient interfacial layer can effectively suppress dendrite growth and ensure ultralong-term stable lithium stripping/plating. This strategy is further demonstrated to provide substantially improved cycle performance in copper current collector, 10 cm2 pouch cell and lithium–sulfur batteries, which, coupled with a simple fabrication process and wide applicability in various materials for lithium-metal protection, makes the lithiophilic–lithiophobic gradient interfacial layer a favored strategy for next-generation lithium-metal batteries.

Li-B alloy has uniform Li deposition morphology and offers better capacity retention as advantageous anode properties over metallic lithium.

No abstract

A multi-core-shell with a conductive network structured C-PANI-S@PANI composite with high sulfur content up to 87% was synthesized. The composite cathode delivers higher specific capacity and excellent cycle stability, retaining a reversible discharge capacity of 835 mA h g(-1) after 100 cycles when the sulfur loading of the cathode was above 6 mg cm(-2).

Nowadays, lithium-ion batteries (LIBs) have been widely used in portable electronics, electric vehicles, and grid energy storage systems. [1][2][3] However, the traditional LIBs based on graphite anode cannot satisfy the ever growing energy density demands. [4,5] In this background, next-generation Li-ion batteries based on Li metal anode with ultrahigh energy density have attracted worldwide attention in recent years, such as lithium-sulfur (2600 Wh kg −1 ), Li-O 2 batteries (3580 Wh kg −1 ). [6][7][8] Li metal anode with high theoretical specific capacity (3860 mAh g −1 ), low density (0.534 g cm −3 ), and the lowest potential (−3.040 V vs standard hydrogen electrode) demonstrated remarkable advantages in energy density as anode for Li metal batteries (LMBs). [9][10][11][12][13][14] However, the practical application of Li metal anode in LMBs is still suffering from low coulombic efficiency (CE), poor cycle life, and safety concerns because of serious Li dendrite growth during cycling. [15][16][17] The uncontrollable dendrite growth leads to the formation of "dead lithium" with low coulombic efficiency, and may even cause catastrophic failure of battery by internal short circuit. [18][19][20] During the past decade, there are majorly two kinds of strategies proposed to suppress dendrite growth and protect lithium metal anode. The first approach is based on a mechanical blocking strategy, such as, 1) optimization of the solid electrolyte interface (SEI) layer and improving its mechanical modulus and stability, for which LiF, [21][22][23] Li 3 N, [24] Li 2 S, [25][26][27] Li 3 PO 4 , [28] Li 2 O, [29] etc. have been introduced into the SEI layer and showed an improved cycling performance at 1.0-2.0 mA cm −2 ; 2) introducing an extra coating layer (poly(dimethylsiloxane), [30] hollow carbon spheres, [31] artificial solid electrolyte layer, [32] etc.) as a protecting layer on the surface of Li metal. The other approach is focused on designing various nanostructures to control the electric field distribution and accommodate volume expansion. In which, hierarchical frameworks such as 3D carbon fiber cloth, [33] Ni foam, [34] and 3D porous Cu foil [35,36] have been constructed to store Li metal and inhibit the growth of Li dendrites. However, these two strategies were both converged at inhibiting lithium deposition, which have not changed the fundamental, self-amplification behavior of the dendrite growth. Moreover, they failed to support the practical application of Li-S or Li-O 2 Uncontrollable Li dendrite growth and low Coulombic efficiency severely hinder the application of lithium metal batteries. Although a lot of approaches have been developed to control Li deposition, most of them are based on inhibiting lithium deposition on protrusions, which can suppress Li dendrite growth at low current density, but is inefficient for practical battery applications, with high current density and large area capacity. Here, a novel leveling mechanism based on accelerating Li growth in concave fashion is proposed, which ena...