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Inside or Outside: Origin of Lithium Dendrite Formation of All Solid-State Electrolytes

机译：内部或外部：所有固态电解质的锂枝晶形成的起源

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摘要

All-solid-state lithium metal batteries (ASSLMBs) stand out for the next generation of energy storage system. However, the further realization is severely hampered by the lithium dendrite formation in solid state electrolytes (SSEs), by mechanisms that remain controversial. Herein, with the aid of experimental and theoretical approaches, the origin of dendrite formation in representative LiBH4 SSE, which is thermodynamically stable with the Li metal, suppressing the side reaction between Li and SSE is elucidated. It is demonstrated that upon diffusion, Li+ encounters an electron, and is subsequently reduced to Li-0 within the grain boundary/pore of SSE, eventually leading to short circuit. Thus, introducing LiF with the ability of interstitial filling and low electronic conductivity into SSE is the effective countermeasure, and as expected, with the addition of LiF, the critical current density (CCD) increases by 235% compared to the value of pure LiBH4. The TiS2|LiBH4-LiF|Li ASSLMBs manifest a reversible capacity of 137 mAh g(-1) at 0.4 C upon 60 cycles. These findings not only unravel critical issues in Li dendrite formation in SSE, but also propose the countermeasure.
机译：全固态锂金属电池（ASSLMB）在下一代储能系统中脱颖而出。但是，由于存在争议的机制，固态电解质（SSE）中锂枝晶的形成严重阻碍了进一步的实现。在此，借助于实验和理论方法，阐明了代表性的LiBH4SSE中的枝晶形成的起源，其对Li金属是热力学稳定的，从而抑制了Li和SSE之间的副反应。结果表明，在扩散时，Li +遇到电子，随后在SSE的晶界/孔中还原为Li-0，最终导致短路。因此，将具有填隙性和低电子传导性的LiF引入SSE是有效的对策，并且正如预期的那样，通过添加LiF，与纯LiBH4的值相比，临界电流密度（CCD）增长了235％。 TiS2 | LiBH4-LiF | Li ASSLMBs在0.4 C下经过60个循环后显示出137 mAh g（-1）的可逆容量。这些发现不仅揭示了上交所锂枝晶形成的关键问题，而且提出了对策。

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