Lithium Salt Combining Fluoroethylene Carbonate Initiates Methyl Methacrylate Polymerization Enabling Dendrite-Free Solid-State Lithium Metal Battery

IF 13 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Energy & Environmental Materials Pub Date : 2024-04-24 DOI:10.1002/eem2.12751
Xue Ye, Jianneng Liang, Baorong Du, Yongliang Li, Xiangzhong Ren, Dazhuan Wu, Xiaoping Ouyang, Qianling Zhang, Jianhong Liu
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Abstract

This work demonstrates a novel polymerization-derived polymer electrolyte consisting of methyl methacrylate, lithium bis(trifluoromethanesulfonyl)imide and fluoroethylene carbonate. The polymerization of MMA was initiated by the amino compounds following an anionic catalytic mechanism. LiTFSI plays both roles including the initiator and Li ion source in the polymer electrolyte. Normally, lithium bis(trifluoromethanesulfonyl)imide has difficulty in initiating the polymerization reaction of methyl methacrylate monomer, a very high concentration of lithium bis(trifluoromethanesulfonyl)imide is needed for initiating the polymerization. However, the fluoroethylene carbonate additive can work as a supporter to facilitate the degree of dissociation of lithium bis(trifluoromethanesulfonyl)imide and increase its initiator capacity due to the high dielectric constant. The as-prepared poly-methyl methacrylate-based polymer electrolyte has a high ionic conductivity (1.19 × 10−3 S cm−1), a wide electrochemical stability window (5 V vs Li+/Li), and a high Li ion transference number ( t Li + ) of 0.74 at room temperature (RT). Moreover, this polymerization-derived polymer electrolyte can effectively work as an artificial protective layer on Li metal anode, which enabled the Li symmetric cell to achieve a long-term cycling performance at 0.2 mAh cm−2 for 2800 h. The LiFePO4 battery with polymerization-derived polymer electrolyte-modified Li metal anode shows a capacity retention of 91.17% after 800 cycles at 0.5 C. This work provides a facile and accessible approach to manufacturing poly-methyl methacrylate-based polymerization-derived polymer electrolyte and shows great potential as an interphase in Li metal batteries.

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结合氟碳乙烯的锂盐引发甲基丙烯酸甲酯聚合,实现无树枝状突起的固态金属锂电池
这项研究展示了一种新型聚合衍生聚合物电解质,它由甲基丙烯酸甲酯、双(三氟甲烷磺酰)亚胺锂和碳酸氟乙烯酯组成。甲基丙烯酸甲酯的聚合是由氨基化合物按照阴离子催化机制引发的。LiTFSI 在聚合物电解质中扮演着引发剂和锂离子源的双重角色。通常,双(三氟甲磺酰)亚胺锂很难引发甲基丙烯酸甲酯单体的聚合反应,需要很高浓度的双(三氟甲磺酰)亚胺锂才能引发聚合反应。然而,由于高介电常数,氟碳酸乙烯添加剂可作为助剂,促进双(三氟甲磺酰基)亚胺锂的解离度并提高其引发能力。所制备的聚甲基丙烯酸甲酯基聚合物电解质具有较高的离子电导率(1.19 × 10-3 S cm-1)、较宽的电化学稳定性窗口(5 V vs Li+/Li)以及室温(RT)下 0.74 的较高锂离子转移数()。此外,这种聚合衍生聚合物电解质还能有效地在锂金属阳极上起到人工保护层的作用,从而使锂离子对称电池在 0.2 mAh cm-2 的条件下实现了 2800 h 的长期循环性能。这项工作为制造基于聚甲基丙烯酸甲酯的聚合衍生聚合物电解质提供了一种简便易行的方法,并显示出作为金属锂电池中间相的巨大潜力。
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来源期刊
Energy & Environmental Materials
Energy & Environmental Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
17.60
自引率
6.00%
发文量
66
期刊介绍: Energy & Environmental Materials (EEM) is an international journal published by Zhengzhou University in collaboration with John Wiley & Sons, Inc. The journal aims to publish high quality research related to materials for energy harvesting, conversion, storage, and transport, as well as for creating a cleaner environment. EEM welcomes research work of significant general interest that has a high impact on society-relevant technological advances. The scope of the journal is intentionally broad, recognizing the complexity of issues and challenges related to energy and environmental materials. Therefore, interdisciplinary work across basic science and engineering disciplines is particularly encouraged. The areas covered by the journal include, but are not limited to, materials and composites for photovoltaics and photoelectrochemistry, bioprocessing, batteries, fuel cells, supercapacitors, clean air, and devices with multifunctionality. The readership of the journal includes chemical, physical, biological, materials, and environmental scientists and engineers from academia, industry, and policy-making.
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