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High-Voltage Li-Ion Full-Cells with Ultralong Term Cycle Life at Elevated Temperature

机译：高温下具有超长循环寿命的高压锂离子全电池

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摘要

In order to meet the ever-growing demand for energy and power densities in rechargeable lithium-ion batteries for electric vehicles, intensive research efforts are focusing on increasing output voltage and maintaining high capacity. However, the trade-off for higher voltage is sacrificing the service life of the batteries, since the detrimentally oxidative degradation on the high-potential cathode side would inevitably poison the whole cell. Thus, optimizing strategies for full-cells must take into account, cathode/anode-electrolyte compatibilities, electrochemical reversibility, and even thermal stability for practical applications, which spurs a hierarchical design for full-cell architecture. Benefitting from its superior oxidative stability, ionic liquid (Li/Pyr(13)TFSI) is employed as catholyte, and equimolar LiTFSI/G(3) complex is used as anolyte due to its high graphite-intercalation-chemistry reversibility. Segregated by a metal-organic-framework-based separator, advantages and drawbacks of each electrolyte systems can be synergistically tuned within their isolated environments. Encouragingly, assembled by this hybrid-electrolytes strategy, a LiNi0.5Mn1.5O4 (5 V-class)/graphite Li-ion full-cell holds an ultrahigh capacity retention rate of 83.8% over 1000 cycles at harsh elevated temperature.
机译：为了满足用于电动车辆的可再充电锂离子电池对能量和功率密度的不断增长的需求，深入的研究工作集中在增加输出电压和保持高容量上。然而，较高电压的折衷牺牲了电池的使用寿命，因为在高电势阴极侧上有害的氧化降解将不可避免地毒害整个电池。因此，针对全电池的优化策略必须考虑到阴极/阳极电解质的相容性，电化学可逆性，甚至是实际应用中的热稳定性，这刺激了全电池架构的分层设计。得益于其出色的氧化稳定性，离子液体（Li / Pyr（13）TFSI）被用作阴极电解液，等摩尔LiTFSI / G（3）络合物由于其高的石墨嵌入化学可逆性而被用作阳极电解液。通过基于金属有机框架的隔板隔离，可以在各自隔离的环境中协同调整每个电解质系统的优缺点。令人鼓舞的是，通过这种混合电解质策略组装而成的LiNi0.5Mn1.5O4（5 V级）/石墨锂离子全电池在苛刻的高温下经过1000次循环后，可保持83.8％的超高容量保持率。

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