Regulating Sodium Deposition Behavior by a Triple-Gradient Framework for High-Performance Sodium Metal Batteries.

An efficient method for the synthesis of a self-supporting carbon framework (denoted Gra-GC-MoSe2) is proposed with a triple-gradient structure-in sodiophilic sites, pore volume, and electrical conductivity-which facilitates the highly efficient regulation of Na deposition. In situ and ex situ measurements, together with theoretical calculations, reveal that the gradient distribution of Se heteroatoms in MoSe2, and its derivatives tailor the sodiophilicity, while the gradient distribution of porous nanostructures homogenizes the Na+ diffusion. Therefore, Na deposition occurs from the bottom to the top of the Gra-GC-MoSe2 framework without dendrite formation. In addition, the gradient in electrical conductivity ensures the stripping process does not lead to dead Na. As a result, a Gra-GC-MoSe2 modified Na anode (Na@Gra-GC-MoSe2) shows impressive cycling stability with a high average Coulombic efficiency in an asymmetric cell. In symmetric cells, it also exhibits a long cycling life of 2000 h with a low polarization voltage and works stably even under a large capacity of 10 mAh cm-2. Moreover, a Na@Gra-GC-MoSe2|| Na3V2(PO4)3 full cell delivers a high energy density with an excellent cycling performance.

N,S-Doped Porous Carbon Nanobelts Embedded with MoS2 Nanosheets as a Self-Standing Host for Dendrite-Free Li Metal Anodes.

Metallic Li is one of the most promising anodes for high-energy secondary batteries. However, the enormous volume changes and severe dendrite formation during the Li plating/stripping process hinder the practical application of Li metal anodes (LMAs). We have developed a sulfate-assisted strategy to synthesize a self-standing host composed of N,S-doped porous carbon nanobelts embedded with MoS2 nanosheets (MoS2 @NSPCB) for use in LMAs. In situ measurements and theoretical calculations reveal that the uniformly distributed MoS2 derivatives within the carbon nanobelts serve as stable lithiophilic sites which effectively homogenize Li nucleation and suppress dendrite formation. In addition, the hierarchical porosity and 3D nanobelt networks ensure fast Li-ion diffusion and accommodate the volume change of Li deposits during the plating/stripping process. As a result, a Li-Li symmetric cell using the MoS2 @NSPCB host operates steadily over 1500 h with an ultralow voltage hysteresis (≈24.2 mV) at 3 mA cm-2 /3 mAh cm-2 . When paired with a LiFePO4 cathode, the current collector-free LMA endows the full cell with a high energy density of 460 Wh kg-1 and good cycling performance (with a capacity retention of ≈70% even after 1600 cycles at 10 C).