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Investigation of Complex Intermediates in Solvent-Mediated Synthesis of Thiophosphate Solid-State Electrolytes
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-12-02 , DOI: 10.1021/acs.jpcc.0c08761 Frank M. Delnick 1 , Guang Yang 1 , Ethan C. Self 1 , Harry M. Meyer 1 , Jagjit Nanda 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2020-12-02 , DOI: 10.1021/acs.jpcc.0c08761 Frank M. Delnick 1 , Guang Yang 1 , Ethan C. Self 1 , Harry M. Meyer 1 , Jagjit Nanda 1
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Lithium thiophosphates represent a promising class of solid Li+ conductors for all-solid-state batteries. Scalable solvent-mediated synthesis routes for several Li–P–S ternary compounds have been reported, but little is known regarding the reaction mechanism of such pathways. This work demonstrates that solvent-mediated synthesis of lithium thiophosphate solid electrolytes from mixtures of Li2S and P2S5 proceeds through a highly soluble P2S62– intermediate. This intermediate exhibits virtually the same Raman spectra in several solvents including acetonitrile, methyl acetate, ethyl acetate, ethyl propionate, dimethoxyethane, tetraethylene glycol dimethyl ether, and tetrahydrofuran. Based on this universal intermediate, a general reaction mechanism is proposed for the solvent-mediated synthesis of several lithium thiophosphates including (LiPS3)n, Li2P2S6, Li7P3S11, and Li3PS4.
中文翻译：
溶剂介导的硫代磷酸盐固态电解质合成中的复杂中间体的研究
硫代磷酸锂代表了一种有前景的全固态电池Li +导体。已经报道了几种Li–P–S三元化合物的可扩展溶剂介导的合成路线，但对于此类途径的反应机理知之甚少。这项工作表明，由Li 2 S和P 2 S 5的混合物进行溶剂介导的硫代磷酸锂固体电解质的合成，是通过高度可溶的P 2 S 6 2–中间。该中间体在几种溶剂（包括乙腈，乙酸甲酯，乙酸乙酯，丙酸乙酯，二甲氧基乙烷，四甘醇二甲醚和四氢呋喃）中表现出几乎相同的拉曼光谱。基于这种通用中间体，提出了一种通用的反应机理，用于溶剂介导的几种硫代磷酸锂的合成，包括（LiPS 3）n，Li 2 P 2 S 6，Li 7 P 3 S 11和Li 3 PS 4。
更新日期：2020-12-17
中文翻译：
溶剂介导的硫代磷酸盐固态电解质合成中的复杂中间体的研究
硫代磷酸锂代表了一种有前景的全固态电池Li +导体。已经报道了几种Li–P–S三元化合物的可扩展溶剂介导的合成路线，但对于此类途径的反应机理知之甚少。这项工作表明，由Li 2 S和P 2 S 5的混合物进行溶剂介导的硫代磷酸锂固体电解质的合成，是通过高度可溶的P 2 S 6 2–中间。该中间体在几种溶剂（包括乙腈，乙酸甲酯，乙酸乙酯，丙酸乙酯，二甲氧基乙烷，四甘醇二甲醚和四氢呋喃）中表现出几乎相同的拉曼光谱。基于这种通用中间体，提出了一种通用的反应机理，用于溶剂介导的几种硫代磷酸锂的合成，包括（LiPS 3）n，Li 2 P 2 S 6，Li 7 P 3 S 11和Li 3 PS 4。
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