Highlights In-situ construction of electrostatic repulsion between MoS 2 interlayers is first proposed to successfully prepare Co-doped monolayer MoS 2 under high vapor pressure. The doped Co atoms radically decrease bandgap and lithium ion diffusion energy barrier of monolayer MoS 2 and can be transformed into ultrasmall Co nanoparticles (~2 nm) to induce strong surface-capacitance effect during conversion reaction. The Co doped monolayer MoS 2 shows ultrafast ion transport capability along with ultrahigh capacity and outstanding cycling stability as lithium-ion-battery anodes. Abstract High theoretical capacity and unique layered structures make MoS 2 a promising lithium-ion battery anode material. However, the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS 2 lead to unacceptable ion transport capability. Here, we propose in-situ construction of interlayer electrostatic repulsion caused by Co 2 + substituting Mo 4+ between MoS 2 layers, which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS 2 , thus establishing isotropic ion transport paths. Simultaneously, the doped Co atoms change the electronic structure of monolayer MoS 2 , thus improving its intrinsic conductivity. Importantly, the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport. Hence, the Co-doped monolayer MoS 2 shows ultrafast lithium ion transport capability in half/full cells. This work presents a novel route for the preparation of monolayer MoS 2 and demonstrates its potential for application in fast-charging lithium-ion batteries. Supplementary Information The online version contains supplementary material available at 10.1007/s40820-023-01042-4.
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