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Revealing the Double-Edged Behaviors of Heteroatom Sulfur in Carbonaceous Materials for Balancing K-Storage Capacity and Stability

机译:揭示碳质材料中杂原子硫的双刃行为,用于平衡K储存能力和稳定性

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摘要

Heteroatoms in the carbon matrix are generally considered as active sites to enhance potassium storage capacity, while their adverse effects on ion batteries remain unclear. Herein, a series of sulfur doped carbon (SCDPx) with adjustable S content and crystallinity are accurately synthesized in the closed autoclave by controlling the ratios of precursors. Electrochemical measurements exhibit that heteroatom sulfur displays double-edged electrochemical activities with a high initial potassium storage capacity but poor cycling stability for carbon anode. Combined with solid-state nuclear magnetic resonance (NMR), catalytic tests, and various ex-situ characterizations, it is demonstrated that abundant S in the carbon would not only form C-S-C bonds, acting as active sites to reversibly adsorb/desorb potassium ions for high capacity, but also significantly catalyze the reduction and decomposition of the electrolyte including KPF6 and ethylene carbonate/diethyl carbonate (EC/DEC) to form thicker solid electrolyte interface (SEI) and degrade electrolyte, resulting in rapid capacity decay. As a result, the optimized sample (SCDP2) with the appropriate sulfur doping content exhibits the best electrochemical performance with high capacity (688.4 mA h g(-1) at 100 mA g(-1)), long-term cycling stability (198.4 mA h g(-1) at 2000 mA g(-1) after 10 000 cycles), and excellent rate capability (238.8 mA h g(-1) at 5000 mA g(-1)).
机译:碳基质中的杂原子通常被认为是活性位点,以提高储存能力,而它们对离子电池的不利影响仍不清楚。这里,通过控制前体的比例,在封闭的高压釜中精确地合成一系列具有可调节的S含量和结晶度的硫掺杂碳(SCDPX)。电化学测量表明,杂原子硫显示出具有高初始钾储存能力的双刃电化学活性,但碳阳极循环稳定性差。结合固态核磁共振(NMR),催化试验和各种前原位特征,证明碳中的丰富S不仅形成CSC键,可作为有源位点,以可逆地吸附/解吸钾离子高容量,但也显着催化电解质的电解质的减少和分解,包括KPF6和碳酸亚乙酯/碳酸亚乙酯(EC / DEC)形成较厚的固体电解质界面(SEI)并降解电解质,导致快速容量衰减。结果,具有适当的硫掺杂含量的优化样品(SCDP2)具有高容量(688.4 mA Hg(-1)的最佳电化学性能(在100mA g(-1)),长期循环稳定性(198.4 mA HG(-1)在1000次循环后的2000 mA g(-1)),优异的速率能力(238.8 mA Hg(-1),5000 mA g(-1))。

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  • 来源
    《Advanced Functional Materials》 |2021年第8期|2006875.1-2006875.10|共10页
  • 作者单位

    Univ Sci & Technol China Dept Appl Chem Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China;

    Univ Sci & Technol China Dept Appl Chem Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China;

    Univ Sci & Technol China Dept Appl Chem Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China;

    Univ Sci & Technol China Dept Appl Chem Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China;

    Univ Sci & Technol China Dept Appl Chem Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China;

    Univ Sci & Technol China Expt Ctr Engn & Mat Sci Hefei 230026 Peoples R China;

    Univ Sci & Technol China Dept Appl Chem Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China;

    Ningo Veken New Energy Technol Co Ltd Ningbo 315800 Zhejiang Peoples R China;

    Univ Sci & Technol China Dept Appl Chem Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China;

    Univ Sci & Technol China Dept Appl Chem Hefei Natl Lab Phys Sci Microscale Hefei 230026 Peoples R China;

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

    active sites; carbonaceous materials; catalytic effects; double#8208; edged behaviors; heteroatom sulfur doping;

    机译:活跃点;碳质材料;催化作用;双重‐边缘行为;杂种硫磺掺杂;

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