Ming-Xi Yu, Xue Zhao, Mi Du, Qi-Long Sun, Xin-Yue Wang, Zi-Hao Wang, Ze Gao, Gui-Ru Sun, Wei Lu, Ming Feng
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The MMA and LiNO<sub>3</sub> work in tandem to produce a polymer/inorganic SEI (PI–SEI) characterized by an outer layer enriched with PMMA–Li short–chain polymers and an inner layer enriched with Li<sub>2</sub>O and Li<sub>3</sub>N inorganics. Unlike the SEI formed by conventional additives, this PI–SEI exhibits higher stability and better Li<sup>+</sup> transfer properties. The presence of short–chain polymers in PI–SEI alters the transport uniformity of Li<sup>+</sup>, facilitating stable cycling of Li || Li cell for over 2000 cycles with a capacity of 1 mAh cm<sup>−2</sup>. Furthermore, these PMMA–Li can chemically adsorb lithium polysulfides (LiPSs), thereby inhibiting Li corrosion by LiPSs, and enabling the capacity of lithium–sulfur batteries to achieve 474.3 mAh g<sup>−1</sup> after 500 cycles at 0.5C. 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引用次数: 0
摘要
固体电解质界面相(SEI)的形成和演化过程对锂金属阳极(LMA)的稳定循环至关重要。利用添加剂调节SEI组分的概念被广泛纳入电解质设计中,因为这些添加剂可以改变LMA表面的锂离子(Li+)沉积行为。然而,传统添加剂的能力有限,只能产生松散和多孔的SEI。在这项研究中,我们提出了一种有机添加剂甲基丙烯酸甲酯(MMA),它通过产生LiTFSI的阴离子或自由基来促进LMA表面的原位聚合。MMA和LiNO3协同作用生成聚合物/无机SEI (PI-SEI),其特征是外层富含PMMA-Li短链聚合物,内层富含Li2O和Li3N无机物。与传统添加剂形成的SEI不同,这种PI-SEI具有更高的稳定性和更好的Li+转移性能。PI-SEI中短链聚合物的存在改变了Li+的输运均匀性,促进Li ||锂电池稳定循环超过2000次,容量为1 mAh cm−2。此外,这些PMMA-Li可以化学吸附锂多硫化物(LiPSs),从而抑制LiPSs对Li的腐蚀,并使锂硫电池在0.5C下循环500次后的容量达到474.3 mAh g−1。本研究提出了一种通过原位聚合生成SEI的策略,为未来液态/固态锂金属电池中LMA的商业化发展提供了支持。图形抽象
In–situ formation of polymer–rich solid electrolyte interphase with methyl methacrylate electrolyte additive stabilizes lithium metal anodes for lithium–sulfur batteries
The formation and evolution process of the solid electrolyte interphase (SEI) is critical for stable cycling of the lithium metal anode (LMA). The concept of regulating SEI components with additives is widely incorporated into electrolyte design, as these additives can alter the lithium ion (Li+) deposition behavior on the surface of LMA. However, conventional additives are limited in their ability to produce only loose and porous SEI. In this study, we propose an organic additive of methyl methacrylate (MMA) that facilitates in-situ polymerization on the surface of LMA by generating anions or free radicals from LiTFSI. The MMA and LiNO3 work in tandem to produce a polymer/inorganic SEI (PI–SEI) characterized by an outer layer enriched with PMMA–Li short–chain polymers and an inner layer enriched with Li2O and Li3N inorganics. Unlike the SEI formed by conventional additives, this PI–SEI exhibits higher stability and better Li+ transfer properties. The presence of short–chain polymers in PI–SEI alters the transport uniformity of Li+, facilitating stable cycling of Li || Li cell for over 2000 cycles with a capacity of 1 mAh cm−2. Furthermore, these PMMA–Li can chemically adsorb lithium polysulfides (LiPSs), thereby inhibiting Li corrosion by LiPSs, and enabling the capacity of lithium–sulfur batteries to achieve 474.3 mAh g−1 after 500 cycles at 0.5C. This study presents a strategy for generating SEI through the in-situ polymerization, which supports the commercial development of LMA in future liquid/solid Li metal batteries.
期刊介绍:
Rare Metals is a monthly peer-reviewed journal published by the Nonferrous Metals Society of China. It serves as a platform for engineers and scientists to communicate and disseminate original research articles in the field of rare metals. The journal focuses on a wide range of topics including metallurgy, processing, and determination of rare metals. Additionally, it showcases the application of rare metals in advanced materials such as superconductors, semiconductors, composites, and ceramics.