Although the meticulous design of functional diversity
within the
polymer interfacial layer holds paramount significance in mitigating
the challenges associated with hydrogen evolution reactions and dendrite
growth in zinc anodes, this pursuit remains a formidable task. Here,
a large-scale producible zinc-enriched/water-lean polymer interfacial
layer, derived from carboxymethyl chitosan (CCS), is constructed on
zinc anodes by integration of electrodeposition and a targeted complexation
strategy for highly reversible Zn plating/stripping chemistry. Zinc
ions-induced crowding effect between CCS skeleton creates a strong
hydrogen bonding environment and squeezes the moving space for water/anion
counterparts, therefore greatly reducing the number of active water
molecules and alleviating cathodic I3
– attack. Moreover, the as-constructed Zn2+-enriched layer
substantially facilitate rapid Zn2+ migration through the
NH2–Zn2+-NH2 binding/dissociation
mode of CCS molecule chain. Consequently, the large-format Zn symmetry
cell (9 cm2) with a Zn-CCS electrode demonstrates excellent
cycling stability over 1100 h without bulging. When coupled with an
I2 cathode, the assembled Zn–I2 multilayer
pouch cell displays an exceptionally high capacity of 140 mAh and
superior long-term cycle performance of 400 cycles. This work provides
a universal strategy to prepare large-scale production and high-performance
polymer crowding layer for metal anode-based battery, analogous outcomes
were veritably observed on other metals (Al, Cu, Sn).