ABSTRACT Aqueous zinc–halogen batteries (ZHBs) offer safety and low cost but are hindered by halogen dissolution, shuttle effects, and sluggish interfacial kinetics. We present a trinity cooperative electrode (TCE) that integrates a conductive polymer, a supramolecular solvent matrix, and an elastic polymer network to simultaneously enhance electronic conductivity, mechanical/solvent stability, and halogen immobilization. The iodine conversion pathway is elucidated by in situ/ex situ characterizations and molecular dynamics simulations. In ZnI 2 + Zn(CF 3 SO 3 ) 2 electrolytes, TCE‐based cells deliver 255 mAh g −1 at 1 A g −1 , retain 150 mAh g −1 at 50 A g −1 for > 50 000 cycles, and operate reliably at −10°C. The TCE also catalyzes Br − /Br 2 conversion in Zn(CF 3 SO 3 ) 2 + ZnBr 2 and enables sequential multielectron reactions in a ternary Zn(CF 3 SO 3 ) 2 + ZnI 2 + ZnBr 2 electrolyte, achieving ∼200 mAh g −1 at 30 A g −1 for > 22 000 cycles. This approach advances high‐energy, long‐life ZHBs through pseudocapacitive interfacial chemistry.
Lai et al. (Mon,) studied this question.