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Design, Synthesis, and Characterization of Polymer Precursors to LixPON and LixSiPON Glasses: Materials That Enable All-Solid-State Batteries (ASBs)
Macromolecules ( IF 5.5 ) Pub Date : 2020-03-20 , DOI: 10.1021/acs.macromol.0c00254
Xinyu Zhang 1 , Eleni Temeche 1 , Richard M. Laine 1
Affiliation  

LiPON-like glasses that form lithium dendrite impenetrable interfaces between lithium battery components are enabling materials that may replace liquid electrolytes permitting production of all-solid-state batteries (ASBs). Unfortunately, to date, such materials are introduced only via gas-phase deposition. Here, we demonstrate the design and synthesis of easily scaled, low-temperature, low-cost, solution-processable inorganic polymers containing LiPON/LiSiPON elements. OPCl3 and hexachlorophosphazene [Cl2P═N]3 provide starting points for elaboration using MNH2 (M = Li/Na) or (Me3Si)NH followed by reaction with controlled amounts of LiNH2 to produce oligomers/polymers with molecular weights (MWs) ≈1–2 kDa characterized by multinuclear NMR, gel permeation chromatography (GPC), thermogravimetric analysis (TGA), Fourier-transform infrared (FTIR), X-ray powder diffraction (XRD), X-ray photoelectron spectroscopy (XPS), and matrix-assisted laser desorption/ionization (MALDI)-time-of-flight (ToF) offering stabilities to 150–200 °C and ceramic yields (800 °C) of 50–60%. 7Li NMR suggests that precursor-bound Li+ dissociates easily, beneficial for electrochemical applications. XPS shows higher N/P ratios (1–3) than via gas-phase methods (<1) correlating N/P ratios, 7Li shifts, and Li+ conductivities. Li2SiPHN offers the highest ambient conductivity of 3 × 10–1 mS cm–1 at 400 °C/2 h/N2.

中文翻译:

Li x PON和Li x SiPON玻璃的聚合物前体的设计,合成和表征:能够实现全固态电池(ASB)的材料

在锂电池组件之间形成锂枝晶无法穿透的界面的类LiPON眼镜使材料可以替代液体电解质,从而可以生产全固态电池(ASB)。不幸的是,迄今为止,这种材料仅通过气相沉积引入。在这里,我们演示了包含LiPON / LiSiPON元素的易于缩放,低温,低成本,可溶液处理的无机聚合物的设计和合成。OPCl 3和六氯磷腈[氯2 P = N] 3提供开始使用MNH阐述点2(M =锂/钠)或(ME 3 Si)的NH接着反应用受控量的灵2生产具有多核NMR,凝胶渗透色谱(GPC),热重分析(TGA),傅立叶变换红外(FTIR),X射线粉末衍射(XRD)表征的分子量(MWs)约1-2 kDa的低聚物/聚合物,X射线光电子能谱(XPS)和基质辅助激光解吸/电离(MALF)飞行时间(ToF)可在150–200°C的温度范围内保持稳定,而陶瓷收率(800°C)在50–60 %。7 Li NMR表明与前体结合的Li +易于解离,对电化学应用有利。XPS显示的N / P比(1-3)高于通过气相法(<1)关联的N / P比,7个Li位移和Li +电导率。李2SiPHN在400°C / 2 h / N 2时具有3×10 –1 mS cm –1的最高环境电导率。
更新日期:2020-04-24
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