Stable sodium anodes for sodium metal batteries (SMBs) enabled by in-situ formed quasi solid-state polymer electrolyte

Huang

ACS Appl. Energy Mater.

et al. 2023

The poor interfacial contact between solid-state electrolytes (SSEs) and electrodes, which hinders the applications of solid-state batteries (SSBs), could be improved by in situ polymerization. However, the limited electrochemical window and insufficient mechanical strength of in situ-polymerized electrolytes make them unable to match high-voltage cathodes and inhibit lithium dendrites. Here, a layered organic–inorganic composite solid-state electrolyte structure is designed by introducing a Li1.3Al0.3Ti1.7(PO4)3 (LATP)-coated polyethylene separator and fluoroethylene carbonate (FEC) into in situ-polymerized 1,3-dioxolane (DOL). The high-voltage stable fluoride-rich cathode–electrolyte interface formed in situ by FEC widens the electrochemical window of the composite solid-state electrolyte. In addition, the LATP coating layer inhibits the growth of lithium dendrites and increases the Li-ion conductivity by reacting with FEC to generate FEC derivatives. The Li/LiCoO2 battery exhibits good cycling and rate performance with a cutoff voltage of 4.3 V at room temperature. It provides a simple and practical solution to improve the performance of high-voltage lithium metal batteries based on in situ polymerization.

Section: Characterization Of Materials and In Situ Polymerizationmentioning

confidence: 98%

Section: Introductionmentioning

confidence: 99%

Layer-Structured Composite Solid-State Electrolyte with a Li_1.3Al_0.3Ti_1.7(PO₄)₃-Coated Separator for High-Voltage Lithium Metal Batteries by In Situ Polymerization

Huang

ACS Appl. Energy Mater.

et al. 2023

Interdisciplinary Materials

“…The utilization of GPE in both S|Li and LiFePO 4 |Li batteries delivered excellent cycling performance for 1000 and 700 cycles, respectively (Figure 2C). In addition to DME, [33][34][35][36] carbonates such as ethylene carbonate (EC), [37] fluoroethylene carbonate (FEC), [38][39][40] and methyl ethyl carbonate [41] have also been studied as cosolvents for DOL in PDOL-based GPEs. Compared with ether solvents, carbonates possess stable thermodynamic properties, high dielectric constant, and low volatility which enable high safety and better anode reversibility.…”

Section: Ethersmentioning

confidence: 99%

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

Xiao

Hao

Bai

et al. 2023

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.

ACS Appl. Mater. Interfaces

“…The negatively charged silicate layers enable facile cation exchange with other ions . LAP has been extensively modified to improve its properties for use in energy storage materials, such as solid-state electrolytes, separators, and binders. ,, 1,3-Dioxolane (DOL) is a cyclic ether that exhibits the potential for polymerization through specific cationic initiators, leading to the formation of poly(1,3-dioxolane) (PDOL) . PDOL has garnered considerable interest due to its high ionic conductivity and good interfacial compatibility with the Li anode. − In addition, the introduction of PDOL modifications to nanoparticles holds the potential to enhance their dispersion.…”

Section: Introductionmentioning

confidence: 99%

“…20,22,24 1,3-Dioxolane (DOL) is a cyclic ether that exhibits the potential for polymerization through specific cationic initiators, leading to the formation of poly(1,3-dioxolane) (PDOL). 25 PDOL has garnered considerable interest due to its high ionic conductivity and good interfacial compatibility with the Li anode. 26−28 In addition, the introduction of PDOL modifications to nanoparticles holds the potential to enhance their dispersion.…”

Section: Introductionmentioning

confidence: 99%

Laponite-Supported Gel Polymer Electrolyte with Multiple Lithium-Ion Transport Channels for Stable Lithium Metal Batteries

Wang

Jin

Huang

et al. 2023

Lithium metal batteries have emerged as a promising candidate for next-generation power systems. However, the high reactivity of lithium metal with liquid electrolytes has resulted in decreased battery safety and stability, which poses a significant challenge. Herein, we present a modified laponitesupported gel polymer electrolyte (LAP@PDOL GPE) that was fabricated using in situ polymerization initiated by a redoxinitiating system at ambient temperature. The LAP@PDOL GPE effectively facilitates the dissociation of lithium salts via electrostatic interaction and simultaneously constructs multiple lithiumion transport channels within the gel polymer network. This hierarchical GPE demonstrates a remarkable ionic conductivity of 5.16 × 10 −4 S cm −1 at 30 °C. Furthermore, the robust laponite component of the LAP@PDOL GPE forms a barrier against Li dendrite growth while also participating in the establishment of a stable electrode/electrolyte interface with Si-rich components. The in situ polymerization process further improves the interfacial contact, enabling the LiFePO 4 /LAP@PDOL GPE/Li cell to exhibit an impressive capacity of 137 mAh g −1 at 1C, with a capacity retention of 98.5% even after 400 cycles. In summary, the developed LAP@PDOL GPE shows great potential in addressing the critical issues of safety and stability associated with lithium metal batteries while also delivering improved electrochemical performance.