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Vanadium-Iodine Co-Regulation Enabled by Trifunctional Conjugated Organic Interface for High-Energy and Robust Zn
Yueyang Wang1, Runze Wang1, Linfeng Yu1
1State Key Laboratory of Chemical Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing, China.
None:
Aqueous Zn batteries (AZBs) utilizing vanadium-iodine dual energy storage mechanisms hold great promise for large-scale energy storage applications. Yet, the development of such AZBs is plagued by severe vanadium dissolution and uncontrolled polyiodide shuttling during the multi-step electron transfer process. Herein, we reported a core-shell VO2 cathode wrapped in situ by a conjugated poly(phenylenediamine) (pPDA) layer, denoted VO2-pPDA, which enables highly reversible and efficient V5+/V4+/V3+ and I-/I0 redox reactions in ZnI2-containing electrolytes. According to in/ex situ characterizations and theoretical calculation results, abundant ─C═N─ moieties in poly(PDA) enabled a synergistic optimization for the stabilization of VO2 and interfacial iodine anchoring. Meanwhile, the π-conjugated framework of poly(PDA) collaborated with VO2 to catalyze the high-efficiency iodine conversion. Due to V-I co-regulation, Zn//VO2-pPDA battery exhibited a high working voltage of 1.09 V, ultrahigh capacity of 610 mAh g-1, and outstanding lifespan over 40 000 cycles. Moreover, a practical 1.0 Ah pouch cell further demonstrated the strong application potential of this system, highlighting the effectiveness of multifunctional interfacial organic engineering for high-performance Zn batteries.
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