Conflicting entropy-driven zwitterionic dry polymer electrolytes for scalable high-energy all-solid-state batteries

Area of Science:

• Materials Science
• Electrochemistry
• Polymer Chemistry

Background:

• Inorganic electrolytes in all-solid-state batteries (ASSBs) present challenges like interfacial instability and complex manufacturing.
• Limitations hinder the commercial viability and scalability of current ASSB technology.

Purpose of the Study:

• To develop a novel zwitterionic dry polymer electrolyte (ZPE) for scalable, energy-dense ASSBs.
• To address interfacial instability and manufacturing complexity associated with inorganic electrolytes.

Main Methods:

• Utilized a conflicting entropy strategy and Flory-Huggins theory to design zwitterionic monomers.
• Achieved in situ polymerization of homogeneous monomer/salt mixtures to form directionally aligned ion channels.
• Integrated ZPEs as solid catholytes into high-areal-capacity LiNi0.8Co0.1Mn0.1O2 electrodes.

Main Results:

• ZPEs demonstrated enhanced salt dissociation and rapid Li+ migration via ion hopping under ambient conditions.
• Full cells achieved high specific energy (516 Wh/kg) and energy density (1329 Wh/L).
• Stable cycling performance was observed at practical operating conditions (25°C, 0.5 MPa).

Conclusions:

• Zwitterionic dry polymer electrolytes offer a transformative solution for next-generation ASSBs.
• The developed ZPEs are compatible with existing manufacturing processes, reducing complexity and cost.
• This approach paves the way for scalable, high-performance, and commercially viable ASSBs.