Inside-Outside Lithium Deposition Achieved by the Unusual Strategy of Constructing the Hierarchical Lithiophilicity for Dendrite-Free and Durable Lithium Metal Anode

Graphical Constructing lithiophilic skeleton : An unusual substrate with heterogeneous lithiophilicity, Ag nanoparticles encapsulated inside nitrogen (N)-doped carbon hollow spheres (denoted as Ag@NCHSs), is demonstrated to induce uniform Li deposition. Uncontrollable dendritic lithium (Li) growth and huge volume fluctuation are critical issues for the commercialization of Li metal anode. This work reports a three-dimensional conductive host with hierarchical lithiophilicity to promote the uniform Li plating/stripping. Except for the common merits of the large surface area and excellent conductivity, the unique structural and compositional design, Ag nanoparticles encapsulated inside nitrogen-doped carbon hollow spheres (Ag@NCHSs), allows a model of inside-outside Li deposition due to the promising lithiophilicity of Ag component. This type of Li deposition strategy is evidenced by in-situ optical microscope, in-situ X-ray diffraction (XRD) patterns and endows a promising ability to overcome the fatal issues of Li metal anode even at high areal capacities and current densities. As a result, the developed host with the hierarchical lithiophilicity enables a remarkable enhancement of cycling performances. The strategy of constructing hierarchical lithiophilicity brings new insights to stabilize the Li metal anode.