Li metal batteries (LMBs) have attracted widespread attention in recent years because of their high energy densities. But traditional LMBs using liquid electrolyte have potential safety hazards, such as: leakage and flammability. Replacing liquid electrolyte with solid polymer electrolyte (SPE) can not only significantly improve the safety, but also improve the energy density of LMBs. However, till now, there is only limited success in improving the various physical and chemical properties of SPE, especially in thickness, posing great obstacles to further promoting its fundamental and applied studies. In this review, the authors mainly focus on evaluating the merits of ultrathin SPE and summarizing its existing challenges as well as fundamental requirements for designing and manufacturing advanced ultrathin SPE in the future. Meanwhile, the authors outline existing cases related to this field as much as possible and summarize them from the perspective of synthetic chemistry, hoping to provide a comprehensive understanding and serve as a strategic guidance for designing and fabricating high-performance ultrathin SPE. Challenges and opportunities regarding this burgeoning field are also critically evaluated at the end of this review.
Li metal anode attracts tremendous attention in next-generation battery systems with high energy density, but volume change and dendritic growth limit its practical applications. Composite Li electrode can fundamentally suppress the volume effect and decrease the local current density, ensuring long-term cycling life. However, up to now, there is only limited success in preparing multifarious composite Li electrode, especially in thickness, posing great obstacles to further promoting its research and application. In this review, the thickness of composite Li electrode are strategically focussed upon and the merits and existing challenges of ultrathin composite Li electrode are evaluated. Meanwhile, the design principles and fundamental requirements for ultrathin composite Li electrode in the future are summarized and the existing cases related to this field are outlined as much as possible from synthetic chemistry, hoping it can serve as a handbook to provide a comprehensive understanding and guide reliable fabrication of advanced composite Li electrode. Challenges and opportunities regarding this burgeoning field are also critically evaluated at the end of this review.
The key to developing high-performance polymer electrolytes (PEs) is to achieve their high strength and high ionic conductivity, but this is still challenging. Herein, we designed a new double-network PE based on the nonhydrolytic sol–gel reaction of tetraethyl orthosilicate and in situ polymerization of zwitterions. The as-prepared PE possesses high strength (0.75 Mpa) and high stretchability (560%) due to the efficient dissipation energy of the inorganic network and elastic characteristics of the polymer network. In addition, the highest ionic conductivity of the PE reaches 0.44 mS cm−1 at 30 °C owning to the construction of dynamic ion channels between the polyzwitterion segments and between the polyzwitterion segments and ionic liquids. Furthermore, the inorganic network can act as Lewis acid to adsorb trace impurities, resulting in a prepared electrolyte with a high electrochemical window over 5 V. The excellent interface compatibility of the as-prepared PE with a Li metal electrode is also confirmed. Our work provides new insights into the design and preparation of high-performance polymer-based electrolytes for solid-state energy storage devices.
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