Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy.

Development of high-energy non-aqueous lithium-sulfur batteries via redox-active interlayer strategy.
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DOI:
10.1038/s41467-022-31943-8
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发表时间:
2022-08-08
影响因子:
16.6
通讯作者:
--
中科院分区:
综合性期刊1区
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--
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锂硫电池的理论比能量高于最先进的锂离子电池。然而,从实际角度来看,由于多硫化物在循环过程中穿梭,这些电池表现出较差的循环寿命和较低的能量含量。为了解决这些问题,研究人员提出在含硫阴极和锂金属阳极之间使用氧化还原惰性保护层。然而,这些夹层给电池带来了额外的重量,从而降低了实际的比能。在这里,我们报告了由硫浸渍的极性有序介孔二氧化硅组成的氧化还原活性中间层的开发和测试。与氧化还原非活性中间层不同,这些氧化还原活性中间层能够实现可溶性多硫化物的电化学再活化,通过二氧化硅-多硫化物极性相互作用保护锂金属电极免受有害反应,并增加电池容量。事实上,当在非水锂硫纽扣电池配置中进行测试时,使用中间层可实现约 8.5 mAh cm−2 的初始放电容量(总硫质量负载为 10mgcm−2),并且在 335mAg−1 和 25°C 下循环 700 次后放电容量保持率约为 64%。锂硫电池有望实现高能量密度,但多硫化物穿梭是实际开发的主要障碍。在这里,提出了一种氧化还原活性夹层来限制多硫化物,增加电池容量并改善电池循环寿命。
Lithium-sulfur batteries have theoretical specific energy higher than state-of-the-art lithium-ion batteries. However, from a practical perspective, these batteries exhibit poor cycle life and low energy content owing to the polysulfides shuttling during cycling. To tackle these issues, researchers proposed the use of redox-inactive protective layers between the sulfur-containing cathode and lithium metal anode. However, these interlayers provide additional weight to the cell, thus, decreasing the practical specific energy. Here, we report the development and testing of redox-active interlayers consisting of sulfur-impregnated polar ordered mesoporous silica. Differently from redox-inactive interlayers, these redox-active interlayers enable the electrochemical reactivation of the soluble polysulfides, protect the lithium metal electrode from detrimental reactions via silica-polysulfide polar-polar interactions and increase the cell capacity. Indeed, when tested in a non-aqueous Li-S coin cell configuration, the use of the interlayer enables an initial discharge capacity of about 8.5 mAh cm−2 (for a total sulfur mass loading of 10 mg cm−2) and a discharge capacity retention of about 64 % after 700 cycles at 335 mA g−1 and 25 °C. Lithium-sulfur batteries promise high energy density, but polysulfide shuttling acts as a major stumbling block toward practical development. Here, a redox-active interlayer is proposed to confine polysulfides, increase the cell capacity and improve cell cycle life.
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