Dynamically Favorable Ion Channels Enabled by a Hybrid Ionic‐Electronic Conducting Film toward Highly Reversible Zinc Metal Anodes

Abstract Aqueous zinc ion batteries show great promise for future applications due to their high safety and ecofriendliness. However, nonuniform dendrite growth and parasitic reactions on the Zn anode have severely impeded their use. Herein, a hybrid ionic‐electronic conducting ink composed of graphene‐like carbon nitride (g‐C 3 N 4 ) and conductive polymers (CP) of poly(3,4ethylenedioxythiophene)‐poly(styrenesulfonate) (PEDOT:PSS) is introduced to Zn anode using a scalable spray‐coating strategy. Notably, the g‐C 3 N 4 promotes a screening effect, disrupting the coulombic interaction between the PEDOT + segments and PSS − chains within CP, thereby reducing interfacial resistance and homogenizing the surface electric field distribution of the Zn anode. Furthermore, the abundant N‐containing species and ─SO 3 − groups in g‐C 3 N 4 /CP exhibit strong zincophilicity, which accelerates the diffusion of Zn 2+ and disrupts the solvation structure of Zn(H 2 O) 6 2+ , thus improving the Zn 2+ transfer capability. Consequently, the g‐C 3 N 4 /CP can powerfully stabilize the Zn 2+ flux and thus enable a high coulombic efficiency of 99.47% for 1500 cycles and smooth Zn plating/stripping behaviors more than 3000 h at a typical current density of 1 mA cm −2 . These findings shed new light on the Zn electrodeposition process under the mediation of g‐C 3 N 4 /CP and offer sustainability considerations in designing more stable Zn‐metal anodes with enhanced reversibility.