Long-Life and High-Power Binder-Free Cathode Based on One-Step Synthesis of Radical Polymers with Multi-Pendant Groups

The main bottlenecks for the widespread application of radical polymers in organic radical batteries are poor cycling stability, due to the dissolution of radical polymers into the electrolyte, and the low efficiency of multi-step synthesis strategies. Herein, a kind of electrolyte-resistant radical polymer bearing multi-pendant groups (poly(ethylene-alt-TEMPO maleate) (PETM)) is designed and synthesized through a one-step esterification reaction to graft 4-hydroxy-2,2,6,6-teramethylpiperidinyl-1-oxy into the commercially available poly(ethylene-alt-maleic anhydride). Interestingly, PETM is hardly soluble in the ethylene carbonate/dimethyl carbonate/ethyl methyl carbonate-based electrolyte, showing an extremely low solubility of 0.59 mg mL(-1), but is easily soluble in tetrahydrofuran and N-Methyl pyrrolidone. The derived binder-free PETM cathode exhibits nearly 100% utilization of the grafted nitroxide radicals (88 mA h g(-1)) and excellent rate capability with almost invariant capacitance from 10 C to 40 C. Significantly, the PETM cathodes retain 94% of the initial capacity after 1000 cycles, outperforming most reported radical polymer-based cathodes.