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Surface Chemistry in Cobalt Phosphide-Stabilized Lithium-Sulfur Batteries

机译:磷酸钴稳定的锂硫电池的表面化学

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摘要

Chemistry at the cathode/electrolyte interface plays an important role for lithium–sulfur batteries in which stable cycling of the sulfur cathode requires confinement of the lithium polysulfide intermediates and their fast electrochemical conversion on the electrode surface. While many materials have been found to be effective for confining polysulfides, the underlying chemical interactions remain poorly understood. We report a new and general lithium polysulfide-binding mechanism enabled by surface oxidation layers of transition-metal phosphide and chalcogenide materials. We for the first time find that CoP nanoparticles strongly adsorb polysulfides because their natural oxidation (forming Co–O–P-like species) activates the surface Co sites for binding polysulfides via strong Co–S bonding. With a surface oxidation layer capable of confining polysulfides and an inner core suitable for conducting electrons, the CoP nanoparticles are thus a desirable candidate for stabilizing and improving the performance of sulfur cathodes in lithium–sulfur batteries. We demonstrate that sulfur electrodes that hold a high mass loading of 7 mg cm~(–2) and a high areal capacity of 5.6 mAh cm~(–2) can be stably cycled for 200 cycles. We further reveal that this new surface oxidation-induced polysulfide-binding scheme applies to a series of transition-metal phosphide and chalcogenide materials and can explain their stabilizing effects for lithium–sulfur batteries.
机译:阴极/电解质界面的化学作用对于锂硫电池起着重要的作用,其中硫阴极的稳定循环需要限制多硫化锂中间体及其在电极表面的快速电化学转化。尽管发现许多材料对限制多硫化物有效,但对潜在的化学相互作用的了解仍然很少。我们报告了一种新的和通用的多硫化锂结合机理,该机理由过渡金属磷化物和硫属化物材料的表面氧化层实现。我们第一次发现CoP纳米颗粒强烈吸附多硫化物,因为它们的自然氧化(形成类似Co–O–P的物质)通过牢固的Co–S键合激活了表面Co位置,从而结合了多硫化物。具有能够限制多硫化物的表面氧化层和适合传导电子的内核,因此CoP纳米颗粒是稳定和改善锂硫电池中硫阴极性能的理想候选材料。我们证明,具有7 mg cm〜(–2)的高质量负载和5.6 mAh cm〜(–2)的高面积容量的硫电极可以稳定地循环200次。我们进一步揭示,这种新的表面氧化诱导的多硫化物结合方案适用于一系列过渡金属磷化物和硫属化物材料,并可以解释它们对锂硫电池的稳定作用。

著录项

  • 来源
    《Journal of the American Chemical Society》 |2018年第4期|1455-1459|共5页
  • 作者单位

    Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States,Energy Sciences Institute, Yale University, West Haven, Connecticut 06516, United States;

    Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China;

    Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States,Energy Sciences Institute, Yale University, West Haven, Connecticut 06516, United States;

    Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States,Energy Sciences Institute, Yale University, West Haven, Connecticut 06516, United States;

    Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States,Energy Sciences Institute, Yale University, West Haven, Connecticut 06516, United States;

    Department of Chemistry, Yale University, New Haven, Connecticut 06520, United States,Energy Sciences Institute, Yale University, West Haven, Connecticut 06516, United States;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);美国《生物学医学文摘》(MEDLINE);美国《化学文摘》(CA);
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  • 正文语种 eng
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  • 入库时间 2022-08-18 03:07:17

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