Walle Kumlachew Zelalem, Musuvadhi Babulal Lakshmipriya, Wu She Huang, Chien Wen-Chen, Jose Rajan, Lue Shingjiang Jessie, Chang Jeng-Kuei, Yang Chun-Chen
Battery Research Center of Green Energy, Ming Chi University of Technology, New Taipei City 24301, Taiwan, R.O.C.
Graduate Institute of Science and Technology, National Taiwan University of Science and Technology, 43, Sec. 4, Keelung Road, Taipei 106, Taiwan, R.O.C.
ACS Appl Mater Interfaces. 2021 Jan 20;13(2):2507-2520. doi: 10.1021/acsami.0c17422. Epub 2021 Jan 6.
Although solid-state Li-metal batteries (LMBs) featuring polymer-based solid electrolytes might one day replace conventional Li-ion batteries, the poor Li-ion conductivity of solid polymer electrolytes at low temperatures has hindered their practical applications. Herein, we describe the first example of using a co-precipitation method in a Taylor flow reactor to produce the metal hydroxides of both the Ga/F dual-doped LiLaZrO (Ga/F-LLZO) ceramic electrolyte precursors and the LiMoO-modified NiCoMnO (LMO@T-LNCM 811) cathode materials for LMBs. The Li/Nafion (LiNf)-coated Ga/F-LLZO (LiNf@Ga/F-LLZO) ceramic filler was finely dispersed in the poly(vinylidene fluoride)/polyacrylonitrile/lithium bis(trifluoromethanesulfonimide)/succinonitrile matrix to give a trilayer composite polymer electrolyte (denoted "Tri-CPE") through a simple solution-casting. The bulk ionic conductivity of the Tri-CPE at room temperature was approximately 4.50 × 10 S cm and exhibited a high Li ion transference number (0.84). It also exhibits a broader electrochemical window of 1-5.04 V Li/Li. A full cell based on a CR2032 coin cell containing the LMO@T-LNCM811-based composite cathode, when cycled under 1 C/1 C at room temperature for 300 cycles, achieved an average Columbic efficiency of 99.4% and a capacity retention of 89.8%. This novel fabrication strategy for Tri-CPE structures has potential applications in the preparation of highly safe high-voltage cathodes for solid-state LMBs.
尽管具有聚合物基固体电解质的固态锂金属电池（LMBs）未来某一天可能会取代传统的锂离子电池，但固体聚合物电解质在低温下较差的锂离子传导率阻碍了它们的实际应用。在此，我们描述了首个在泰勒流反应器中使用共沉淀法制备用于LMBs的Ga/F双掺杂LiLaZrO（Ga/F-LLZO）陶瓷电解质前驱体以及LiMoO改性的NiCoMnO（LMO@T-LNCM 811）阴极材料的金属氢氧化物的实例。通过简单的溶液浇铸，将Li/Nafion（LiNf）包覆的Ga/F-LLZO（LiNf@Ga/F-LLZO）陶瓷填料精细分散在聚偏二氟乙烯/聚丙烯腈/双（三氟甲烷磺酰）亚胺锂/丁二腈基体中，得到一种三层复合聚合物电解质（称为“Tri-CPE”）。Tri-CPE在室温下的本体离子传导率约为4.50×10 S cm，并且表现出高锂离子迁移数（0.84）。它还具有更宽的1 - 5.04 V Li/Li电化学窗口。基于CR2032硬币电池的全电池，包含基于LMO@T-LNCM811的复合阴极，在室温下以1 C/1 C循环300次时，平均库仑效率达到99.4%，容量保持率为89.8%。这种用于Tri-CPE结构的新型制备策略在制备用于固态LMBs的高安全性高压阴极方面具有潜在应用。
