An Ion‐Pumping Quasi‐Solid Electrolyte Enabled by Electrokinetic Effects for Stable Aqueous Zinc Metal Batteries

Abstract The practical application of aqueous zinc (Zn) metal batteries (ZMBs) is hindered by the complicated hydrogen evolution, passivation reactions, and dendrite growth of Zn metal anodes. Here, an ion‐pumping quasi‐solid electrolyte (IPQSE) with high Zn 2+ transport kinetics enabled by the electrokinetic phenomena to realize high‐performance quasi‐solid state Zn metal batteries (QSSZMBs) is reported. The IPQSE is prepared through the in situ ring‐opening polymerization of tetramethylolmethane‐tri‐β‐aziridinylpropionate in the aqueous electrolyte. The porous polymer framework with high zeta potential provides the IPQSE with an electrokinetic ion‐pumping feature enabled by the electrokinetic effects (electro‐osmosis and electrokinetic surface conduction), which significantly accelerates the Zn 2+ transport, reduces the concentration polarization and overcomes the diffusion‐limited current. Moreover, the Zn 2+ affinity of the polymer and hydrogen bonding interactions in the IPQSE changes the Zn 2+ coordination environment and reduces the amount of free H 2 O, which lowers the H 2 O activity and inhibits H 2 O‐induced side reactions. Consequently, the highly reversible and stable Zn metal anodes are achieved. The assembled QSSZMBs based on the IPQSE display excellent cycling stability with high capacity retention and Coulombic efficiency. The high‐performance quasi‐solid state Zn metal pouch cells are demonstrated, showing great promise for the practical application of the IPQSE.