Abstract

Composite polymer electrolytes (CPEs) incorporate the advantages of solid polymer electrolytes (SPEs) and inorganic solid electrolytes (ISEs), which have shown huge potential in the application of safe lithium-metal batteries (LMBs). Effectively avoiding the agglomeration of inorganic fillers in the polymer matrix during the organic–inorganic mixing process is very important for the properties of the composite electrolyte. Herein, a partial cross-linked PEO-based CPE was prepared by porous vinyl-functionalized silicon (p-V-SiO2) nanoparticles as fillers and poly (ethylene glycol diacrylate) (PEGDA) as cross-linkers. By combining the mechanical rigidity of ceramic fillers and the flexibility of PEO, the as-made electrolyte membranes had excellent mechanical properties. The big special surface area and pore volume of nanoparticles inhibited PEO recrystallization and promoted the dissolution of lithium salt. Chemical bonding improved the interfacial compatibility between organic and inorganic materials and facilitated the homogenization of lithium-ion flow. As a result, the symmetric Li|CPE|Li cells could operate stably over 450 h without a short circuit. All solid Li|LiFePO4 batteries were constructed with this composite electrolyte and showed excellent rate and cycling performances. The first discharge-specific capacity of the assembled battery was 155.1 mA h g−1, and the capacity retention was 91% after operating for 300 cycles at 0.5 C. These results demonstrated that the chemical grafting of porous inorganic materials and cross-linking polymerization can greatly improve the properties of CPEs.

Highlights

  • Nowadays, the urgent demands for green energy and high-energy storage systems promote the high-speed development of rechargeable energy storage devices [1,2,3,4,5]

  • Lithium-metal batteries (LMBs) with solid-state electrolytes (SSEs) have higher specific capacity and more stable electrochemical stability, and they can be used in wearable electronic devices [11,15,16]

  • Absorption peaks shifted to left thealong left along thethe absorption peaks shifted to the with with a decrease of the intensity, p-V-SiO

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Summary

Introduction

The urgent demands for green energy and high-energy storage systems promote the high-speed development of rechargeable energy storage devices [1,2,3,4,5]. There are serious safety issues in traditional commercialized lithium-ion batteries, as the use of liquid electrolyte has the shortcomings of leakage, flammability, and toxicity [9]. With the inevitable trend of upgrading lithium-ion batteries, solid-state electrolytes (SSEs) show huge potential in enhancing the safety performance of LIBs and have been researched extensively [10]. SSEs make it possible to use the Li metal, which possesses high theoretical capacity (3680 mA h g−1 ) and the lowest electrochemical potential (−3.04 V vs standard hydrogen electrode) as an anode electrode in lithium battery [11,12,13,14]. Lithium-metal batteries (LMBs) with SSEs have higher specific capacity and more stable electrochemical stability, and they can be used in wearable electronic devices [11,15,16]

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