4.8 Article

Realizing Spherical Lithium Deposition by In Situ Formation of a Li2S/Li-Sn Alloy Mixed Layer on Carbon Paper for Stable and Safe Li Metal Anodes

Journal

ACS APPLIED MATERIALS & INTERFACES
Volume 13, Issue 41, Pages 48828-48837

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsami.1c14889

Keywords

mixed Li2S/Li-Sn coating; low diffusion energy barrier; lithiophilic Li-Sn alloy; spherical lithium deposition; dendrite-free Li metal anode

Funding

  1. National Natural Science Foundation of China [21805182]
  2. Shanghai Engineering Research Center of Intelligent Computing System [19DZ2252600]

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The study utilized uniform SnS2 nanosheets coated on a carbon paper skeleton to form a mixed layer of Li2S/Li-Sn, allowing for homogeneous Li deposition and inhibiting the formation of Li dendrites, resulting in improved cycle life and Coulombic efficiency of the electrode.
Uncontrollable formation of Li dendrites and volume expansion have always been serious obstacles to the practical application of Li metal anodes. Three-dimensional (3D) frameworks are proven to accommodate Li to suppress volume expansion, but the lithiophobic surface tends to cause uncontrollable formation of Li dendrites. Here, uniform SnS2 nanosheets are coated on the carbon paper (SnS2@CP) skeleton and then transformed into a mixed layer of Li2S/Li-Sn after lithiation. Under the joint action of the lithiophilic Li-Sn alloy and low-diffusion energy barrier Li2S, the dual effects of strong adsorption and rapid diffusion of Li are realized. As a result, Li deposits homogeneously within the whole framework; as the plating amount increases, dendritefree spherical Li is demonstrated, and the thickness of the electrode stays almost unchanged even at a high areal capacity of 10 mA h cm(-2). The SnS2@CP electrodes present an ultralow nucleation overpotential (ca. 4 mV), high Coulombic efficiency (above 96.6% for more than 450 cycles), and stable cycle life (>1500 h), indicating that the 3D framework with the Li2S/Li-Sn alloy mixed coating has excellent lithiophilicity and fast Li transport kinetics, thus effectively inhibiting the formation of Li dendrites. All the findings give new insights into the design strategy for stable and safe Li metal anodes.

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