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yexuqing木蟲(chóng)之王 (文學(xué)泰斗)
太陽(yáng)系系主任
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[交流]
Li2ZrF6-based electrolytes for durable lithium metal batteries
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Li2ZrF6-based electrolytes for durable lithium metal batteries 用于耐用鋰金屬電池的Li2ZrF6基電解質(zhì) ▲ 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 ▲ 鏈接：https://www.nature.com/articles/s41586-024-08294-z ▲ 摘要：鋰（Li）金屬電池（MNB）是一種很有前途的高能量密度可充電電池。然而，由高活性鋰和非水電解質(zhì)之間的反應(yīng)形成的鋰枝晶導(dǎo)致了安全性問(wèn)題和快速的容量衰減。開(kāi)發(fā)可靠的固體電解質(zhì)界面對(duì)于實(shí)現(xiàn)高速率和長(zhǎng)壽命的LMB至關(guān)重要，但在技術(shù)上仍然具有挑戰(zhàn)性。 研究者證明了在含有LiPF6的LMB碳酸鹽電解質(zhì)中添加過(guò)量的m-Li2ZrF6（單斜晶體的）納米顆粒，有助于在施加電壓的驅(qū)動(dòng)下將大量的ZrF62 -離子釋放到電解質(zhì)中，轉(zhuǎn)化為t-Li2ZrF6（三方晶系），并在原位形成穩(wěn)定的固體-電解質(zhì)界面，具有高鋰離子電導(dǎo)率。 計(jì)算電鏡和低溫透射電鏡研究表明，富m-Li2ZrF6固電解質(zhì)界面的原位形成顯著增強(qiáng)了鋰離子的轉(zhuǎn)移，抑制了鋰枝晶的生長(zhǎng)。結(jié)果表明，采用LiFePO4陰極、三維鋰碳陽(yáng)極和Li2ZrF6基電解質(zhì)組裝的lmb在3000次循環(huán)后具有較高的容量保持率（>80.0%），大大提高了循環(huán)穩(wěn)定性。這一成就代表了領(lǐng)先的性能，因此在實(shí)際的高速率條件下，為耐用的LMB提供了可靠的基于Li2ZrF6的電解質(zhì)。 ▲ 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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