Electrode

Organic chemistry

Covalent bond

Polymer chemistry

Ethylene oxide

Polyurethane

Reagent

Network covalent bonding

Ionic conductivity

Engineering

Physical chemistry

Copolymer

Ionic bonding

Chemistry

Salt (chemistry)

Materials science

Imide

Prepolymer

Electrolyte

Chemical engineering

Polymer

Chemistry of Materials

Mechanically durable polymer network electrolytes are desirable for batteries; however, covalent cross-linking adversely affects their large-scale manufacturing, and they are difficult to recycle post-lifespan. Here, we address the electrolyte reprocessability and recyclability challenges through the use of dynamic covalent bonds for polymer network solid electrolytes. Specifically, the associative dynamic vinylogous urethane motif is incorporated into a poly(ethylene oxide) network electrolyte containing lithium bis(fluorosulfonyl)imide (LiFSI) salt. The resulting dynamic covalent network electrolyte possesses a modest ion conductivity (∼10–5 S/cm at room temperature) and good reprocessability. Stress–relaxation studies indicate that the LiFSI salt can catalyze the bond exchange and enhance the network dynamics. Furthermore, the reprocessability associated with bond exchange can be tuned by simply adjusting the formulation of reagent compositions, in which increasing the amount of excess amine or using a shorter chain of PEO prepolymer can further enhance the network dynamics and corresponding reprocessability.

Reprocessable and Recyclable Polymer Network Electrolytes via Incorporation of Dynamic Covalent Bonds