Fast lithium ion transport with a high current density is critical for thick sulfur cathodes, stemming mainly from the difficulties in creating effective lithium ion pathways in high sulfur content electrodes. To develop a high-rate cathode for lithium-sulfur (Li-S) batteries, extenuation of the lithium ion diffusion barrier in thick electrodes is potentially straightforward. Here, a phyllosilicate material with a large interlamellar distance is demonstrated in high-rate cathodes as high sulfur loading. The interlayer space (≈1.396 nm) incorporated into a low lithium ion diffusion barrier (0.155 eV) significantly facilitates lithium ion diffusion within the entire sulfur cathode, and gives rise to remarkable nearly sulfur loading-independent cell performances. When combined with 80% sulfur contents, the electrodes achieve a high capacity of 865 mAh g at 1 mA cm and a retention of 345 mAh g at a high discharging/charging rate of 15 mA cm , with a sulfur loading up to 4 mg. This strategy represents a major advance in high-rate Li-S batteries via the construction of fast ions transfer paths toward real-life applications, and contributes to the research community for the fundamental mechanism study of loading-independent electrode systems.

The growing demand for lithium batteries with higher energy densities requires new electrode chemistries. Lithium metal is a promising candidate as the anode material due to its high theoretical specific capacity, negative electrochemical potential and favorable density. However, during cycling, low and uneven lithium ion concentration on the surface of anode usually results in uncontrolled dendrite growth, especially at high current densities. Here we tackle this issue by using lithiophilic montmorillonite as an additive in the ether-based electrolyte to regulate the lithium ion concentration on the anode surface and thus facilitate the uniform lithium deposition. The lithiophilic montmorillonite demonstrates a pumping feature that improves the self-concentrating kinetics of the lithium ion and thus accelerates the lithium ion transfer at the deposition/electrolyte interface. The signal intensity of TFSI− shows negligible changes via in situ Raman tracking of the ion flux at the electrochemical interface, indicating homogeneous ion distribution, which can lead to a stable and uniform lithium deposition on the anode surface. Our study indicates that the interfacial engineering induced by the lithiophilic montmorillonite could be a promising strategy to optimize the lithium deposition for next-generation lithium metal batteries.

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