Active Oxygenated Group-Rich Polymer Electrolyte Synchronizing Bilateral Interfacial Stabilization and Accelerated...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Commercialization of high-energy-density solid-state lithium-oxygen batteries (SSLOBs) is limited by poor interfacial compatibility and slow cathodic kinetics.
• Solid-solid contact in conventional electrolytes leads to performance degradation and hinders practical application.

Purpose of the Study:

• To develop an innovative polymer electrolyte that simultaneously enhances interfacial compatibility and accelerates cathodic reaction kinetics in SSLOBs.
• To overcome the limitations of current SSLOB technology for high-performance energy storage.

Main Methods:

• Synthesis of a polymerized glycidyl methacrylate (PGM) electrolyte featuring abundant active oxygenated groups (AOGs).
• Investigation of PGM's effect on Li+ solvation structure and solid electrolyte interphase (SEI) formation on Li metal anode.
• Utilizing theoretical calculations to understand the role of AOGs in stabilizing lithium-oxygen intermediates and facilitating Li2O2 decomposition.
• Fabrication and electrochemical testing of PGM-based lithium-oxygen batteries (PGM-LOBs).

Main Results:

• The PGM electrolyte successfully modulated the Li+ solvation structure, leading to a dense, oxide-rich SEI that suppressed Li dendrite growth.
• AOGs in the PGM electrolyte stabilized lithium-oxygen intermediates and lowered the energy barrier for Li2O2 decomposition, enhancing oxygen reaction kinetics.
• PGM-LOBs demonstrated a high capacity of 13,076 mAh g-1 at 200 mA g-1, a low overpotential of 0.56 V, and stable cycling for 150 cycles (1500 h).
• In ambient air, PGM-LOBs exhibited stable cycling for 400 h with a discharge capacity of 19,044 mAh g-1 at 200 mA g-1.

Conclusions:

• The developed AOG-rich PGM polymer electrolyte is a viable strategy for simultaneously improving interfacial compatibility and oxygen redox kinetics in SSLOBs.
• This approach paves the way for advanced, high-performance SSLOBs with enhanced safety and energy density.
• The study highlights the potential of tailored polymer electrolytes in next-generation battery technologies.