Elucidating the Impact of Functional Additives on the Structure and Ion Dynamics of Hybrid Solid Electrolytes
S. Zhang (TU Delft - RST/Storage of Electrochemical Energy)
Yuhang Li (Tsinghua University)
Lars J. Bannenberg (TU Delft - RID/TS/Instrumenten groep)
Ming Liu (Tsinghua University)
M Wagemaker (TU Delft - RST/Storage of Electrochemical Energy)
S Ganapathy (TU Delft - RST/Storage of Electrochemical Energy, TU Delft - RID/TS/Instrumenten groep)
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Abstract
One of the major challenges in advancing polymer-inorganic hybrid solid electrolytes (HSEs) lies in comprehending and controlling their internal structure. In addition, the intricate interplay between multiple phases further complicates efforts to establish the structure-property relationships. In this study, by introducing a multifunctional LiI additive to an HSE compromising of polyethylene oxide (PEO) polymeric electrolyte and the fast lithium-ion conductor Li6PS5Cl, the relationship between the bulk and interface structure and ascertaining their impact on lithium-ion dynamics within the HSE is disentangled. Using multidimensional solid-state nuclear magnetic resonance, we find that the addition of LiI stabilizes the internal interfaces and enhances lithium-ion mobility. A kinetically stable solid-electrolyte interphase is formed at the lithium-metal anode, increasing the critical current density to 1.3 mA cm−2, and enabling long-term stable cycling of lithium symmetric cells (>1200 h). This work sheds light on tailoring the structure of HSEs to improve their conductivity and stability for enabling all-solid-state lithium-metal batteries.
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