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Research Article

Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature

Jieshuangyang Chen1,§, Jie Lei2,§, Jinwei Zhou1, Xuanfeng Chen1, Rongyu Deng1, Mingzhi Qian1, Ya Chen1( ), Feixiang Wu1( )
School of Metallurgy and Environment, Engineering Research Center of the Ministry of Education for Advanced Battery Materials, Hunan Provincial Key Laboratory of Nonferrous Value-added Metallurgy, Central South University, Changsha 410083, China
College of Materials Science and Engineering, Institute of New Energy Materials and Engineering, Fuzhou University, Fuzhou 350108, China

§ Jieshuangyang Chen and Jie Lei contributed equally to this work.

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Graphical Abstract

A novel catalyst NiCo-MoOx/rGO (rGO = reduced graphene oxides) is developed to simultaneously present the superior adsorption ability and excellent catalytic activity without the limitation of Sabatier effect, achieving high-performance Li-S batteries with wide operating temperature from −20 to 60 °C.

Abstract

The development of electrocatalysts with high catalytic activity is conducive to enhancing polysulfides adsorption and reducing activation energy of polysulfides conversion, which can effectively reduce polysulfide shuttling in Li-S batteries. Herein, a novel catalyst NiCo-MoOx/rGO (rGO = reduced graphene oxides) with ultra-nanometer scale and high dispersity is derived from the Anderson-type polyoxometalate precursors, which are electrostatically assembled on the multilayer rGO. The catalyst material possesses dual active sites, in which Ni-doped MoOx exhibits strong polysulfide anchoring ability, while Co-doped MoOx facilitates the polysulfides conversion reaction kinetics, thus breaking the Sabatier effect in the conventional electrocatalytic process. In addition, the prepared NiCo-MoOx/rGO modified PP separator (NiCo-MoOx/rGO@PP) can serve as a physical barrier to further inhibit the polysulfide shuttling effect and realize the rapid Li+ migration. The results demonstrate that Li-S coin cell with NiCo-MoOx/rGO@PP separator shows excellent cycling performance with the discharge capacity of 680 mAh·g−1 after 600 cycles at 1 C and the capacity fading of 0.064% per cycle. The rate performance is also impressive with the remained capacity of 640 mAh·g−1 after 200 cycles even at 4 C. When the sulfur loading is 4.0 mg·cm−2 and electrolyte volume/sulfur mass ratio (E/S) ratio is 6.0 μL·mg−1, a specific capacity of 830 mAh·g−1 is achieved after 200 cycles with a capacity decay of 0.049% per cycle. More importantly, the cell with NiCo-MoOx/rGO@PP separator exhibits cycling performance under wide operating temperature with the reversible capacities of 518, 715, and 915 mAh·g−1 after 100 cycles at −20, 0, and 60 °C, respectively. This study provides a new design approach of highly efficient catalysts for sulfur conversion reaction in Li-S batteries.

Keywords

lithium-sulfur batteriesdoped molybdenum oxideseparator modificationadsorption and catalysis dual-siteswide temperature

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Nano Research
Volume 17 Issue 11,
November 2024
Pages 9651-9661
DOI: 10.1007/s12274-024-6879-8
Cite this article:
Chen J, Lei J, Zhou J, et al. Polysulfides adsorption and catalysis dual-sites on metal-doped molybdenum oxide nanoclusters for Li-S batteries with wide operating temperature. Nano Research, 2024, 17(11): 9651-9661. https://doi.org/10.1007/s12274-024-6879-8
Topics:
CatalyticLithium batteriesTransition metals

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Received: 16 May 2024
Revised: 03 July 2024
Accepted: 11 July 2024
Published: 16 August 2024
© Tsinghua University Press 2024
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