Li, Y., Wang, W., Zhang, B., Fu, L., Wan, M., Li, G., Cai, Z., Tu, S., Duan, X., Seh, Z. W., Jiang, J., & Sun, Y. (2021). Manipulating Redox Kinetics of Sulfur Species Using Mott–Schottky Electrocatalysts for Advanced Lithium–Sulfur Batteries. Nano Letters, 21(15), 6656–6663. https://doi.org/10.1021/acs.nanolett.1c02161
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 Li2S 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–1 under high S loading (10.73 mg cm–2) and lean electrolyte (E/S = 5.9 μL mgsulfur–1) 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.
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Publisher Copyright
Funding Info:
This research / project is supported by the Singapore National Research Foundation - NRF Fellowship
Grant Reference no. : NRF-NRFF2017-04
Overseas Funding:-
1) National Natural Science Foundation of China (No. 52002136, 51802105)
2) Innovation Fund of Wuhan National Laboratory for Optoelectronics of Huazhong University of Science and Technology.
3) China Postdoctoral Science Foundation (No. 2020M682400)
4) China Postdoctoral Science Foundation (No.2018M640694, 2020T130223)