A specific free-volume network as synergistic zinc–ion–conductor interface towards stable zinc anode

The rechargeable aqueous zinc (Zn) ion battery is considered to be the most promising battery due to its inherent safety, low cost and high capacity. However, the Zn anode suffers from the low Coulombic efficiency (CE), irreversible dendritic growth and side reactions. Herein, we separate aqueous electrolyte from Zn anode by coating polymers of intrinsic microporosity (PIMs) layer, which possess unique rigid framework and abundant free volume and provide plentiful storage sites and ordered transport channels for Zn2+. The specific protective structure of PIM-1 endows the Zn anode with an extremely low nucleation overpotential of 8 mV, and enables a [email protected]//Cu asymmetric battery to achieve a high average CE of 99.7% for 500 cycles. The [email protected] symmetric battery achieves stability for over 2500 h at a current density of 0.5 mA cm−2. The capacity of [email protected]/NH4V4O10 full battery can still reach 170 mAh g − 1 after 9500 cycles at 10 A g − 1. Moreover, the transmission mechanism of Zn2+through OO path in PIM-1 is elucidated by density functional theory (DFT) calculations. This work opens a new avenue for the application of uniform porous polymers in the field of high-performance aqueous batteries.