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yexuqing木虫之王 (文学泰斗)
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Li2ZrF6-based electrolytes for durable lithium metal batteries
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Li2ZrF6-based electrolytes for durable lithium metal batteries 用于耐用锂金属电池的Li2ZrF6基电解质 ▲ 作者：Qingshuai Xu, Tan Li, Zhijin Ju, Guangxu Chen, Daiqi Ye, Geoffrey I. N. Waterhouse, Yingying Lu, Xuejun Lai, Guangmin Zhou, Lin Guo, Keyou Yan, Xinyong Tao, Hong Li & Yongcai Qiu ▲ 链接：https://www.nature.com/articles/s41586-024-08294-z ▲ 摘要：锂（Li）金属电池（MNB）是一种很有前途的高能量密度可充电电池。然而，由高活性锂和非水电解质之间的反应形成的锂枝晶导致了安全性问题和快速的容量衰减。开发可靠的固体电解质界面对于实现高速率和长寿命的LMB至关重要，但在技术上仍然具有挑战性。 研究者证明了在含有LiPF6的LMB碳酸盐电解质中添加过量的m-Li2ZrF6（单斜晶体的）纳米颗粒，有助于在施加电压的驱动下将大量的ZrF62 -离子释放到电解质中，转化为t-Li2ZrF6（三方晶系），并在原位形成稳定的固体-电解质界面，具有高锂离子电导率。 计算电镜和低温透射电镜研究表明，富m-Li2ZrF6固电解质界面的原位形成显著增强了锂离子的转移，抑制了锂枝晶的生长。结果表明，采用LiFePO4阴极、三维锂碳阳极和Li2ZrF6基电解质组装的lmb在3000次循环后具有较高的容量保持率（>80.0%），大大提高了循环稳定性。这一成就代表了领先的性能，因此在实际的高速率条件下，为耐用的LMB提供了可靠的基于Li2ZrF6的电解质。 ▲ Abstract：Lithium (Li) metal batteries (LMBs) are promising for high-energy-density rechargeable batteries. However, Li dendrites formed by the reaction between highly active Li and non-aqueous electrolytes lead to safety concerns and rapid capacity decay. Developing a reliable solid–electrolyte interphase is critical for realizing high-rate and long-life LMBs, but remains technically challenging. Here we demonstrate that adding excess m-Li2ZrF6 (monoclinic) nanoparticles to a commercial LiPF6-containing carbonate electrolyte of LMBs facilitates the release of abundant ZrF62– ions into the electrolyte driven by the applied voltage, converting to t-Li2ZrF6 (trigonal) and creating a stable solid–electrolyte interphase in situ with high Li-ion conductivity. Computational and cryogenic transmission electron microscopy studies revealed that the in situ formation of the t-Li2ZrF6-rich solid–electrolyte interphase markedly enhanced Li-ion transfer and suppressed the growth of Li dendrites. As a result, LMBs assembled with LiFePO4 cathodes (areal loading, 1.8/2.2 mAh cm-2), three-dimensional Li–carbon anodes (50- m-thick Li) and Li2ZrF6-based electrolyte displayed greatly improved cycling stability with high capacity retention (>80.0%) after 3,000 cycles (1C/2C rate). This achievement represents leading performance and, thus, delivers a reliable Li2ZrF6-based electrolyte for durable LMBs under practical high-rate conditions. |
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