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Abstract To address the structural instability and rapid capacity fading of the cathodes for aqueous zinc‐ion batteries (AZIBs), a composite cathode material noted as VO‐ i ‐HEC is fabricated in this work by the intercalation of hydroxyethyl cellulose (HEC) into layered vanadium pentoxide (V 2 O 5 ). The electrostatic interactions from the polar functional groups of HEC expand the interlayer spacing of V 2 O 5 from 4.3 to 12.74 Å and cleave V─O (2) ─V bridging bonds, resulting in high‐density lattice defects within VO‐ i ‐HEC. The structural modifications synergistically create pathways for rapid Zn 2+ diffusion and introduce additional redox‐active sites in VO‐ i ‐HEC as well. As a result, VO‐ i ‐HEC achieves a high specific capacity of 499.88 mAh·g⁻ 1 at 0.1 A·g −1 and demonstrates remarkable stability over 2000 cycles at 10 A·g −1 , with a low capacity decay rate of 0.004%. Differential charge density analysis and density functional theory calculations reveal that HEC intercalation enhances electron delocalization, reduces Zn 2+ migration barriers from 0.74 to 0.14 eV, and suppresses parasitic reactions, proving that the structure‐interface synergistic regulation strategy is a highly effective design paradigm for vanadium‐based cathodes in high‐performance AZIBs.
Lu et al. (Sat,) studied this question.