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DOI:
10.1021/acs.macromol.0c00254
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发表时间:
2020
期刊:
影响因子:
5.5
通讯作者:
Laine, R. M.
中科院分区:
文献类型:
--
作者:
Zhang, X.;Temeche, E.;Laine, R. M.
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. OPCl3and hexachlorophosphazene [Cl2P═N]3provide starting points for elaboration using MNH2(M = Li/Na) or (Me3Si)NH followed by reaction with controlled amounts of LiNH2to 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 × 10–1mS cm–1at 400 °C/2 h/N2.