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Enhanced catalysis of radical-to-polysulfide interconversion via increased sulfur vacancies in lithium-sulfur batteries.

ABSTRACT: The practical application of lithium-sulfur (Li-S) batteries is seriously hindered by severe lithium polysulfide (LiPS) shuttling and sluggish electrochemical conversions. Herein, the Co₉S₈/MoS₂ heterojunction as a model cathode host material is employed to discuss the performance improvement strategy and elucidate the catalytic mechanism. The introduction of sulfur vacancies can harmonize the chemisorption of the heterojunction component. Also, sulfur vacancies induce the generation of radicals, which participate in a liquidus disproportionated reaction to reduce the accumulation of liquid LiPSs. To assess the conversion efficiency from liquid LiPSs to solid Li₂S, a new descriptor calculated from basic cyclic voltammetry curves, nucleation transformation ratio, is proposed.

SUBMITTER: Xu R

PROVIDER: S-EPMC9159087 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Enhanced catalysis of radical-to-polysulfide interconversion via increased sulfur vacancies in lithium-sulfur batteries.

Xu Rui R Tang Hongan H Zhou Yuanyuan Y Wang Fangzheng F Wang Hongrui H Shao Minhua M Li Cunpu C Wei Zidong Z

Chemical science 20220510 21

The practical application of lithium-sulfur (Li-S) batteries is seriously hindered by severe lithium polysulfide (LiPS) shuttling and sluggish electrochemical conversions. Herein, the Co9S8/MoS2 heterojunction as a model cathode host material is employed to discuss the performance improvement strategy and elucidate the catalytic mechanism. The introduction of sulfur vacancies can harmonize the chemisorption of the heterojunction component. Also, sulfur vacancies ...[more]

PMID: 35733903

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Project description:The shuttling effect of soluble lithium polysulfides (LiPSs) and the sluggish conversion kinetics of polysulfides into insoluble Li2S2/Li2S severely hinders the practical application of Li-S batteries. Advanced catalysts can capture and accelerate the liquid-solid conversion of polysulfides. Herein, we try to make use of bismuth tantalum oxide with oxygen vacancies as an electrocatalyst to catalyze the conversion of LiPSs by reducing the sulfur reduction reaction (SRR) nucleation energy barrier. Oxygen vacancies in Bi4TaO7 nanoparticles alter the electron band structure to improve instinct electronic conductivity and catalytic activity. In addition, the defective surface could provide unsaturated bonds around the vacancies to enhance the chemisorption capability with LiPSs. Hence, a multidimensional carbon (super P/CNT/Graphene) standing sulfur cathode is prepared by coating oxygen vacancies Bi4TaO7-x nanoparticles, in which the multidimensional carbon (MC) with micropores structure can host sulfur and provide a fast electron/ion pathway, while the outer-coated oxygen vacancies with Bi4TaO7-x with improved electronic conductivity and strong affinities for polysulfides can work as an adsorptive and conductive protective layer to achieve the physical restriction and chemical immobilization of lithium polysulfides as well as speed up their catalytic conversion. Benefiting from the synergistic effects of different components, the S/C@Bi3TaO7-x coin cell cathode shows superior cycling and rate performance. Even under a high level of sulfur loading of 9.6 mg cm-2, a relatively high initial areal capacity of 10.20 mAh cm-2 and a specific energy density of 300 Wh kg-1 are achieved with a low electrolyte/sulfur ratio of 3.3 µL mg-1. Combined with experimental results and theoretical calculations, the mechanism by which the Bi4TaO7 with oxygen vacancies promotes the kinetics of polysulfide conversion reactions has been revealed. The design of the multiple confined cathode structure provides physical and chemical adsorption, fast charge transfer, and catalytic conversion for polysulfides.

Dataset Information

Enhanced catalysis of radical-to-polysulfide interconversion via increased sulfur vacancies in lithium-sulfur batteries.

Publications

Enhanced catalysis of radical-to-polysulfide interconversion <i>via</i> increased sulfur vacancies in lithium-sulfur batteries.

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