Unraveling the Synergistic Coupling Mechanism of Li⁺ Transport in an “Ionogel‐in‐Ceramic” Hybrid Solid Electrolyte for Rechargeable Lithium Metal Battery

Abstract

Understanding the ionic transport behaviors in hybrid solid electrolytes (HSEs) is critically important for the practical realization of rechargeable Li‐metal batteries (LMBs) with high safety. Herein, it is reported a new solid “Ionogel‐in‐Ceramic” electrolyte by using the Li1.3Al0.3Ti1.7(PO4)3 (LATP) ceramic particles as a framework and “Poly(ionic liquid)s‐in‐Salt” (“PolyIL‐in‐Salt”) ionogel as an ionic bridge via a simple pressing process. The “PolyIL‐in‐Salt” ionogel precursor is designed to improve the chemical compatibility at solid–solid interfaces. Molecular dynamics simulations reveal the roles of salt concentrations on the distribution of co‐coordination of “PolyIL‐in‐Salt” ionogel. Moreover, the “PolyIL‐in‐Salt” ionogel containing co‐coordination not only inhibits the parasitic reactions between LATP and Li anode but also provides efficient Li+ conducting pathways. Benefiting from the designed structure, the “Ionogel‐in‐Ceramic” HSE exhibits an excellent ionic conductivity of 0.17 mS cm−1 at 50 °C. Meanwhile, the as‐formed solid electrolyte enables a long cycle of over 3500 h in Li/Li symmetric cell. Further, all‐solid‐state lithium metal batteries fabricated on LiFePO4 and high voltage LiCoO2 cathodes deliver 160.0 mAh g−1, 125.0 mAh g−1, respectively. This study sheds light on the rational design of solid‐state electrolytes with efficient interparticle Li+ conduction, compatible, stable, compact, and durable electrode–electrolyte interfaces.

Rechargeable Iron-Ion Battery Using a Pure Ionic Liquid Electrolyte

“…The proposed working mechanism of the Fe-ion battery is due to the movement of Fe 3+ between the cathode and anode during the charge and discharge processes. This mechanism is similar to Li + movement in Li-ion batteries during the charge and discharge processes. , …”

“…This mechanism is similar to Li + movement in Li-ion batteries during the charge and discharge processes. 17 , 18 …”

“…This mechanism is similar to Li + movement in Li-ion batteries during the charge and discharge processes. 17,18 Charge and Discharge of Full Cell. A charge and discharge test of a full Fe-ion battery was performed.…”

Tough Ionogels: Synthesis, Toughening Mechanisms, and Mechanical Properties─A Perspective

“…e ., high vacuum, low or high temperature). Furthermore, ionogels also show great potential in sensors, energy storage devices, soft robotics, and flexible electronics (Figure b). − …”

“…The tan colored outer band shows properties that lead to applications, of which several are highlighted on the periphery. Applications in (b) were reproduced with permission from ref ( 25 ) (Copyright 2021 Wiley-VCH), ref ( 26 ) (Copyright 2021 Wiley-VCH), ref ( 27 ) (Copyright 2021 Wiley-VCH), and ref ( 28 ) (Copyright 2022 Wiley-VCH).…”