Abstract
Polymer coatings are promising candidates as artificial interfacial materials due to their significant barrier properties and zincophilicity, whereas modified zinc anodes for high depth of discharge (DOD) remain a major challenge. Herein, we present a novel approach that combines electrostatic complexation with phase separation in a weak-acid solution, which induces the formation of acid-responsive porous polyelectrolyte membranes, leading to an extended lifespan of the zinc anode of up to 900 h at a high current density of 40 mA cm(-2). Additionally, the Zn@PEI-PSSNa anode demonstrates excellent zinc utilization, operating for up to 200 h at an ultra-high DOD of 97.3%. The Zn@PEI-PSSNa‖Cu cell further exhibits long-term cycling stability with a super-high coulombic efficiency (CE) of 99.8% for nearly 4000 h. Experimental analysis and simulations indicate that the sulfonate and amino functional groups, along with the porous structure, could improve zincophilicity and facilitate the transport of Zn(2+), thereby promoting uniform zinc deposition, accelerating the desolvation process and mitigating side reactions.