Progress and perspectives of in situ polymerization method for lithium‐based batteries

Abstract

The application of lithium-based batteries is challenged by the safety issues of leakage and flammability of liquid electrolytes. Polymer electrolytes (PEs) can address issues to promote the practical use of lithium metal batteries.However, the traditional preparation of PEs such as the solution-casting method requires a complicated preparation process, especially resulting in side solvents evaporation issues. The large thickness of traditional PEs reduces the energy density of the battery and increases the transport bottlenecks of lithium-ion. Meanwhile, it is difficult to fill the voids of electrodes to achieve good contact between electrolyte and electrode. In situ polymerization appears as a facile method to prepare PEs possessing excellent interfacial compatibility with electrodes. Thus, thin and uniform electrolytes can be obtained. The interfacial impedance can be reduced, and the lithium-ion transport throughput at the interface can be increased. The typical in situ polymerization process is to implant a precursor solution containing monomers into the cell and then in situ solidify the precursor under specific initiating conditions, and has been widely applied for the preparation of PEs and battery assembly. In this review, we focus on the preparation and application of in situ polymerization method in gel polymer electrolytes, solid polymer electrolytes, and composite polymer electrolytes, in which different kinds of monomers and reactions for in situ polymerization are discussed. In addition, the various compositions and structures of inorganic fillers, and their effects on the electrochemical properties are summarized. Finally, challenges and perspectives for the practical application of in situ polymerization methods in solidstate lithium-based batteries are reviewed.

Advanced Electrolytes for Rechargeable Lithium Metal Batteries with High Safety and Cycling Stability

“…In situ polymerization is one of the most common forms of in situ solidification. 12 Compared with traditional liquid electrolytes, in situ polymerized electrolytes exhibit enhanced safety since combustible solvent molecules are polymerized into higher molecular weight polymers, which are fire-retardant. Therefore, in situ polymerization has gained much attention in recent years.…”

“…As illustrated in Figure a, the liquid electrolyte is injected in the pouch cells and infiltrates the electrodes, then is transformed in situ into solid-state. In situ polymerization is one of the most common forms of in situ solidification . Compared with traditional liquid electrolytes, in situ polymerized electrolytes exhibit enhanced safety since combustible solvent molecules are polymerized into higher molecular weight polymers, which are fire-retardant.…”

“…The hybrid solid–liquid electrolytes (HSLEs) combine the benefits of both solid and liquid electrolytes, enhancing the safety and stability of the electrolyte while maintaining a stable interfacial connection . In recent research, in situ solidification has emerged as a popular approach for fabricating solid-state batteries. , Its primary advantage lies in its compatibility with the existing liquid battery production process, facilitating efficient in situ solid–liquid conversion and ensuring excellent contact at the solid–solid interface within the battery. As depicted in Figure , to enhance the safety and stability of LIBs at the electrolyte level, it is imperative to consider factors such as thermal stability, chemical stability, electrochemical stability, flammability, interface stability, compatibility with metallic lithium, and compatibility with cathode materials.…”

Bridging the gap from single molecule properties to organic semiconductor materials

“…The Kondo effect, which is caused by unpaired electrons in radicals 34–38 and metal complexes, can be utilized to determine whether a molecule contains spins in single-molecule devices. 39,40 In addition, the Kondo effect can be finely tuned by the Zeeman effect, which causes the splitting of the energy levels of spin electrons when a magnetic field is applied to the molecule.…”

A Hierarchical Metal–Organic Framework Composite Aerogel Catalyst Containing Integrated Acid, Base, and Metal Sites for the One-Pot Catalytic Synthesis of Cyclic Carbonates

“…Cyclic carbonates (CCs) are high value-added chemicals that have numerous applications in polymerization reactions, lithium-ion batteries, and the preparation of cosmetics and pharmaceuticals. − In this context, direct conversion of alkenes and CO 2 to CCs has attracted great interest owing to its high atom economy and the reduction in the levels of greenhouse gases. Typically, one-pot synthesis of a CC from styrene and CO 2 involves a two-step process, involving a selective oxidation reaction of styrene to form the corresponding epoxide and then subsequent cycloaddition of the epoxide with CO 2 to generate the CCs.…”