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Synergistic Regulation of Polysulfides Conversion and Deposition by MOF-Derived Hierarchically Ordered Carbonaceous Composite for High-Energy Lithium-Sulfur Batteries

机译:MOF衍生的高能锂硫电池多级有序碳质复合材料对多硫化物转化和沉积的协同调控

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摘要

To achieve a high sulfur loading is critical for high-energy lithium-sulfur batteries. However, high sulfur loading, especially at a low electrolyte/sulfur ratio (E/S), usually causes low sulfur utilization, mainly caused by the slow redox kinetics of polysulfides and the passivation of the discharge product, poor electrically/ionically conducting Li2S. Herein, by using cobalt-based metal organic frameworks (Co-MOFs) as precursors, a Co, N-doped carbonaceous composite (Co, N-CNTs (carbon nanotubes)-CNS (carbon nanosheet)/CFC (carbon fiber cloth)) is fabricated with hierarchically ordered structure, which consists of a free-standing 3D carbon fiber skeleton decorated with a vertical 2D carbon nanosheets array rooted by interwoven 1D CNTs. As an effective polysulfides host, the hierarchically ordered 3D conductive network with abundant active sites and voids can effectively trap polysulfides and provide fast electron/ions pathways to convert them. In addition, Co and N heteroatoms can strengthen the interaction with polysulfides and accelerate its reaction kinetics. More importantly, the interwoven CNTs with Co, N-doping can induce 3D Li2S deposition instead of conventional 2D deposition, which benefits improving sulfur utilization. Therefore, for Co, N-CNTs-CNS/CFC electrodes, even at a high sulfur loading of 10.20 mg cm(-2) with a low E/S of 6.94, a high reversible areal capacity of 7.42 mAh cm(-2) can be achieved with excellent cycling stability.
机译:对于高能锂硫电池而言,实现高硫负荷至关重要。但是,高硫负荷,特别是在低电解质/硫比率(E / S)下,通常会导致硫利用率低,这主要是由于多硫化物的氧化还原动力学较慢和放电产物的钝化,电/离子传导性差的Li2S所致。在本文中,通过使用钴基金属有机骨架(Co-MOF)作为前驱体,制成了掺有Co,N的碳质复合物(Co,N-CNT(碳纳米管)-CNS(碳纳米片)/ CFC(碳纤维布))该产品以分层有序的结构制造,由独立的3D碳纤维骨架组成,骨架上装饰有以交织的1D CNT为根的垂直2D碳纳米片阵列。作为有效的多硫化物宿主,具有丰富的活性位点和空隙的分层有序3D导电网络可以有效地捕获多硫化物,并提供快速的电子/离子路径进行转化。另外,Co和N杂原子可以增强与多硫化物的相互作用并加速其反应动力学。更重要的是,具有Co,N掺杂的交织CNT可以诱导3D Li2S沉积,而不是传统的2D沉积,这有利于提高硫的利用率。因此,对于Co,N-CNTs-CNS / CFC电极,即使在高硫负载量为10.20 mg cm(-2)和低E / S为6.94的情况下,其高可逆面容量仍为7.42 mAh cm(-2)可以实现出色的循环稳定性。

著录项

  • 来源
    《Advanced Functional Materials》 |2019年第19期|1900875.1-1900875.11|共11页
  • 作者单位

    Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Beijing Key Lab Ion Liquid Clean Proc, Beijing 100190, Peoples R China|Univ Chinese Acad Sci, Sch Chem & Engn, Beijing 100049, Peoples R China;

    Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Beijing Key Lab Ion Liquid Clean Proc, Beijing 100190, Peoples R China|Univ Chinese Acad Sci, Sch Chem & Engn, Beijing 100049, Peoples R China;

    Northwest A&F Univ, Minist Educ, Key Lab Agr Soil & Water Engn Arid & Semiarid Are, Yangling 712100, Shaanxi, Peoples R China;

    Tianjin Univ Technol, Sch Mat Sci & Engn, Inst New Energy Mat & Low Carbon Technol, Tianjin Key Lab Adv Funct Porous Mat, Tianjin 300384, Peoples R China;

    Beijing Jiaotong Univ, Sch Sci, Minist Educ, Key Lab Luminescence & Opt Informat, Beijing 100044, Peoples R China|Tianjin Univ, Dept Chem, Tianjin Key Lab Mol Optoelect Sci, Tianjin 300072, Peoples R China|Collaborat Innovat Ctr Chem Sci & Engn Tianjin, Tianjin 300072, Peoples R China;

    Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Beijing Key Lab Ion Liquid Clean Proc, Beijing 100190, Peoples R China|Univ Chinese Acad Sci, Sch Chem & Engn, Beijing 100049, Peoples R China;

    Chinese Acad Sci, Inst Proc Engn, CAS Key Lab Green Proc & Engn, Beijing Key Lab Ion Liquid Clean Proc, Beijing 100190, Peoples R China|Univ Chinese Acad Sci, Sch Chem & Engn, Beijing 100049, Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    3D Li2S deposition; carbonaceous composite; high energy; lithium-sulfur batteries; metal-organic frameworks;

    机译:3D Li2S沉积;含碳复合材料;高能;锂硫电池;金属有机骨架;

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