Synergistic regulation of polysulfides shuttle effect and lithium dendrites from cobalt-molybdenum bimetallic carbides (Co-Mo-C) heterostructure for robust Li-S batteries

IF 9.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Chinese Chemical Letters Pub Date : 2024-11-01 DOI:10.1016/j.cclet.2024.110604
Xuanyang Jin, Xincheng Guo, Siyang Dong, Shilan Li, Shengdong Jin, Peng Xia, Shengjun Lu, Yufei Zhang, Haosen Fan
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Abstract

Lithium-sulfur batteries (LSBs) are considered as the most promising energy storage technologies owing to their large theoretical energy density (2500 Wh/kg) and specific capacity (1675 mAh/g). However, the heavy shuttle effect of polysulfides and the growth of lithium dendrites greatly hinder their further development and commercial application. In this paper, cobalt-molybdenum bimetallic carbides heterostructure (Co6Mo6C2@Co@NC) was successfully prepared through chemical etching procedure of ZIF-67 precursor with sodium molybdate and the subsequent high temperature annealing process. The obtained dodecahedral Co6Mo6C2@Co@NC with hollow and porous structure provides large specific surface area and plentiful active sites, which speeds up the chemisorption and catalytic conversion of polysulfides, thus mitigating the shuttle effect of polysulfides and the generation of lithium dendrites. When applied as the LSBs separator modifier layer, the cell with modified separator present excellent rate capability and durable cycling stability. In particular, the cell with Co6Mo6C2@Co@NC/PP separator can maintain the high capacity of 738 mAh/g at the current density of 2 C and the specific capacity of 782.6 mAh/g after 300 cycles at 0.5 C, with the coulombic efficiency (CE) near to 100%. Moreover, the Co6Mo6C2@Co@NC/PP battery exhibits the impressive capacity of 431 mAh/g in high sulfur loading (4.096 mg/cm2) at 0.5 C after 200 cycles. This work paves the way for the development of bimetallic carbides heterostructure multifunctional catalysts for durable Li-S battery applications and reveals the synergistic regulation of polysulfides and lithium dendrites through the optimization of the structure and composition.

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钴钼双金属碳化物(Co-Mo-C)异质结构对多硫化物穿梭效应和锂枝晶的协同调控,用于制造坚固的锂-S 电池
锂硫电池(LSB)因其较大的理论能量密度(2500 Wh/kg)和比容量(1675 mAh/g)而被认为是最有前途的储能技术。然而,多硫化物的重穿梭效应和锂枝晶的生长极大地阻碍了它们的进一步发展和商业应用。本文利用钼酸钠对 ZIF-67 前驱体进行化学蚀刻,随后进行高温退火处理,成功制备了钴钼双金属碳化物异质结构(Co6Mo6C2@Co@NC)。得到的十二面体 Co6Mo6C2@Co@NC 具有中空多孔结构,具有较大的比表面积和丰富的活性位点,可加速多硫化物的化学吸附和催化转化,从而减轻多硫化物的穿梭效应和锂枝晶的生成。作为 LSBs 隔膜改性层,改性隔膜电池具有出色的速率能力和持久的循环稳定性。其中,采用 Co6Mo6C2@Co@NC/PP 隔膜的电池在电流密度为 2 C 时可保持 738 mAh/g 的高容量,在 0.5 C 下循环 300 次后可保持 782.6 mAh/g 的比容量,库仑效率(CE)接近 100%。此外,Co6Mo6C2@Co@NC/PP 电池在 0.5 摄氏度、高硫含量(4.096 毫克/平方厘米)条件下循环 200 次后,显示出 431 毫安时/克的惊人容量。这项工作为开发双金属碳化物异质结构多功能催化剂用于耐用锂-S 电池应用铺平了道路,并通过优化结构和组成揭示了多硫化物和锂枝晶的协同调节作用。
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来源期刊
Chinese Chemical Letters
Chinese Chemical Letters 化学-化学综合
CiteScore
14.10
自引率
15.40%
发文量
8969
审稿时长
1.6 months
期刊介绍: Chinese Chemical Letters (CCL) (ISSN 1001-8417) was founded in July 1990. The journal publishes preliminary accounts in the whole field of chemistry, including inorganic chemistry, organic chemistry, analytical chemistry, physical chemistry, polymer chemistry, applied chemistry, etc.Chinese Chemical Letters does not accept articles previously published or scheduled to be published. To verify originality, your article may be checked by the originality detection service CrossCheck.
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