Manipulating Redox Kinetics of Sulfur Species Using Mott-Schottky Electrocatalysts for Advanced Lithium-Sulfur Batteries.

Li, Yuanjian; Wang, Wenyu; Zhang, Bao; Fu, Lin; Wan, Mintao; Li, Guocheng; Cai, Zhao; Tu, Shuibin et al. · Nano Lett · 2021

basic_science · Level V

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Abstract

Lithium-sulfur (Li-S) batteries suffer from sluggish sulfur redox reactions under high-sulfur-loading and lean-electrolyte conditions. Herein, a typical Co@NC heterostructure composed of Co nanoparticles and a semiconductive N-doped carbon matrix is designed as a model Mott-Schottky catalyst to exert the electrocatalytic effect on sulfur electrochemistry. Theoretical and experimental results reveal the redistribution of charge and a built-in electric field at the Co@NC heterointerface, which are critical to lowering the energy barrier of polysulfide reduction and Li<sub>2</sub>S oxidation in the discharge and charge process, respectively. With Co@NC Mott-Schottky catalysts, the Li-S batteries display an ultrahigh capacity retention of 92.1% and a system-level gravimetric energy density of 307.8 Wh kg<sup>-1</sup> under high S loading (10.73 mg cm<sup>-2</sup>) and lean electrolyte (E/S = 5.9 μL mg<sub>sulfur</sub><sup>-1</sup>) conditions. The proposed Mott-Schottky heterostructure not only deepens the understanding of the electrocatalytic effect in Li-S chemistry but also inspires a rational catalyst design for advanced high-energy-density batteries.