The tightly connected structure of polybenzimidazole (PBI) membrane can be relaxed by solvent/nonsolvent solution to achieve a high proton conductivity for vanadium redox flow battery (VRFB). However, the nature behind the solvent/nonsolvent strategy is not unraveled. This work proposes a guideline to analyze the effect of PBI membrane relaxing formulas based on the interactions between different components in membranes. The supreme-efficient PBI membrane derived by the DMSO/formamide formula according to the guideline displays a marvelous performance for VRFB, with the proton conductivity boosted by 4300% (from 1.93 to 83.33 mS cm-1), and VRFB assembled with this membrane achieves an outstanding energy efficiency of 82.5% under 200 mA cm-2. Moreover, this work profoundly unravels the structure, property and performance relationship of PBI membrane, which is of great value for the development of membranes.
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