In response to prepare high-stable and ion-conducting polyelectrolyte for hydroxide exchange membrane (HEM) applications, we present an ultrastable polyelectrolyte based on six-membered heterocyclic 6-azonia-spiro[5.5]undecane (ASU) and polyphenyl ether (PPO). A series of ASU-functionalized PPO polyelectrolytes (ASU-PPO), which can be easily dissolved in low-boiling pointing solvent, have been successfully synthesized by a remote-grafting method. The ASU precursor is stable in 1 M NaOH/DO at 80 °C for 2500 h as well as in 5 M NaOH/DO at 80 °C for 2000 h, and the predicted half-life of the ASU precursor would exceed 10 000 h, even higher in the future. Besides, these remote-grafting ASU-PPO polyelectrolytes are stable in 1 M NaOH at 80 °C for 1500 h. Robust and pellucid segmented ASU and triple-ammonium-functionalized PPO-based HEMs attach OH conductivity of 96 mS/cm at 80 °C and realize maximal power density of 178 mW/cm under current density of 401 mA/cm.

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