Abstract

The urgent demands for high-energy-density rechargeable batteries promote a flourishing development of Li metal anode. However, the uncontrollable dendrites growth and serious side reactions severely limit its commercial application. Herein, an artificial LiF-rich solid electrolyte interphase (SEI) is constructed at molecular-level using one-step photopolymerization of hexafluorobutyl acrylate based solution, where the LiF is in situ generated during photopolymerization process (denoted as PHALF). The LiF-rich layer comprised flexible polymer matrix and inorganic LiF filler not only ensures intimate contact with Li anode and adapts volume fluctuations during cycling but also regulates Li deposition behavior, enabling it to suppress the dendrite growth and block side reactions between the electrolyte and Li metal. Accordingly, the PHALF-Li anode presents superior stable cycling performance over 500 h at 1 mA·cm⁻² for 1 mA·h·cm⁻² without dendrites growth in carbonate electrolyte. The work provides a novel approach to design and build in situ artificial SEI layer for high-safety and stable Li metal anodes.

中文翻译：

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原位氟化固体电解质向长寿命锂金属阳极过渡

摘要

对高能量密度可充电电池的迫切需求促进了锂金属负极的蓬勃发展。但是，无法控制的枝晶生长和严重的副反应严重限制了其商业应用。本文中，使用六氟丙烯酸丁酯基溶液的一步光聚合，在分子水平上构建了人造富LiF固体电解质中间相（SEI）。在光聚合过程中产生（称为PHALF）。富含LiF的层包括柔性聚合物基体和无机LiF填料，不仅确保与Li阳极紧密接触并适应循环过程中的体积波动，还调节Li的沉积行为，从而能够抑制枝晶生长并阻止电解质与Li之间的副反应。金属。因此，PHALF-Li阳极在1mA·h·cm ^-2下在1mA·cm ^-2的条件下在500h内表现出优异的稳定循环性能，而不会在碳酸盐电解质中产生树枝状生长。这项工作提供了一种新颖的方法来设计和建造用于高安全性和稳定锂金属阳极的原位人工SEI层。