Entropy-Driven Ultrafast Ion Conduction Via Confining Organic Plastic Crystals in Ordered Nanochannels of Covalent Organic Frameworks |
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Authors: | Jing Wang Lili Liu Yukun Liu Xian-Ming Zhang Juan Li |
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Affiliation: | Institute of Crystalline Materials, Shanxi University, Wucheng Rd, No 92, Taiyuan, 030006 China |
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Abstract: | Low conductivity over a wide temperature region due to ultra-slow ion migration dynamics is a key issue in the field of solid-state electrolytes (SSE), which needs to be solved and improved. Covalent organic frameworks (COFs), a rapidly growing class of porous crystalline materials, emerge as a new research hotspot in the field of SSEs. This is due to their homogeneously dispersed sites and well-defined pathways for ion diffusion, demonstrating great advantages over conventional non-porous solids. Herein, a composite solid electrolyte by confining organic ionic plastic crystal (OIPC) in the 1D ordered nanochannels of COFs as the host matrix for solid-state lithium-ion conduction, is reported. Due to the loss of coupling between PBu4+ cations and TFSI− anions, the cation–anion interaction is weakened; and thus, the lithium-ion transportation is facilitated. As a result, the COF-confining OIPC SSEs show ultra-high lithium-ion conductivity of 0.048 S cm−1 at 30 °C and 0.021 S cm−1 at the extremely low temperature of −30 °C. The dynamic origin of this fast ion conduction is characterized by differential scanning calorimetry (DSC), X-ray photoelectron spectroscopy (XPS), and variable temperature solid-state nuclear magnetic resonance (NMR) spectroscopy. |
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Keywords: | covalent organic frameworks lithium ion conductors organic ionic plastic crystals solid state electrolytes |
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