Simultaneous Modulation on Solvation Shell and Electrode Interface for Reversible Zinc Anode Realized by a Mutiplefunctional Additive

Abstract The inferior reversibility of Zn metal anode caused by undesired Zn dendrite and severe interfacial side reactions has to be addressed for the commercial application of Zinc ion batteries (ZIBs). Here, a multiple functional sodium benzaldehyde 2,4‐disulfonate(B24DADS) additives with various blocks of polar sulfonate group, Lewis basic aldehyde groups, and hydrophobic benzene ring is proposed to regulate the solvation structure of Zn2+, construct an H2O‐poor and zincophilic dual electric layer structure, and create a passive SEI on the Zn anode surface, thus restaining dendrite growth and interfacial side reactions. Furthermore, uniform deposition mechanics of the Zn are revealed by the synergistic effect of induced deposition, additive‐derived SEI formation, and texture regulation. In addition, Na+ can also limit the growth of zinc dendrites based on electrostatic shielding mechanisms. Therefore, the multifunctional B24DADS additive grants the anode to deliver remarkable electrochemical performance. Under critical test conditions (20 mA cm−2/20 mAh cm−2), the zinc provides superior long cycling (3700 h) with a low polarization voltage (0.02 V). B24DADS containing electrolyte is well matched with manganese dioxide cathode. This effort renders a promising way to explore advanced additives with unique molecular structures for addressing zinc dendrite growth and rampant side effects.