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Highlights: The amphipathic phenylalanine-adsorbed layer contributes to form a nucleophilic–hydrophobic interface that homogenizes Zn2+ flux while repelling H2O molecules from contacting Zn anode. The preferential reduction of phenylalanine (Phe) prior to H2O facilitates in situ formation of an organic–inorganic hybrid solid electrolyte interphase, enhancing the interfacial stability. Benefiting from the triple protection of Phe, the Zn||Zn and Zn||LMO cells display significantly improved electrochemical performances, even at extreme diluted electrolytes. Aqueous Zn2+-ion batteries (AZIBs), recognized for their high security, reliability, and cost efficiency, have garnered considerable attention. However, the prevalent issues of dendrite growth and parasitic reactions at the Zn electrode interface significantly impede their practical application. In this study, we introduced a ubiquitous biomolecule of phenylalanine (Phe) into the electrolyte as a multifunctional additive to improve the reversibility of the Zn anode. Leveraging its exceptional nucleophilic characteristics, Phe molecules tend to coordinate with Zn2+ ions for optimizing the solvation environment. Simultaneously, the distinctive lipophilicity of aromatic amino acids empowers Phe with a higher adsorption energy, enabling the construction of a multifunctional protective interphase. The hydrophobic benzene ring ligands act as cleaners for repelling H2O molecules, while the hydrophilic hydroxyl and carboxyl groups attract Zn2+ ions for homogenizing Zn2+ flux. Moreover, the preferential reduction of Phe molecules prior to H2O facilitates the in situ formation of an organic–inorganic hybrid solid electrolyte interphase, enhancing the interfacial stability of the Zn anode. Consequently, Zn||Zn cells display improved reversibility, achieving an extended cycle life of 5250 h. Additionally, Zn||LMO full cells exhibit enhanced cyclability of retaining 77.3% capacity after 300 cycles, demonstrating substantial potential in advancing the commercialization of AZIBs. [ABSTRACT FROM AUTHOR]

The Zn//V2O5 system not only faces the incontrollable growth of zinc (Zn) dendrites, but also withstands the cross‐talk effect of by‐products produced from the cathode side to the Zn anode, inducing interelectrode talk and aggravating battery failure. To tackle these issues, we construct a rapid Zn2+‐conducting hydrogel electrolyte (R‐ZSO) to achieve Zn deposition modulation and side reaction inhibition in Zn//V2O5 full cells. The polymer matrix and BN exhibit a robust anchoring effect on SO42−, accelerating Zn2+ migration and enabling dense Zn deposition behavior. Therefore, the Zn//Zn symmetric cells based on the R‐ZSO electrolyte can operate stably for more than 1500 h, which is six times higher than that of cells employing the blank electrolyte. More importantly, the R‐ZSO hydrogel electrolyte effectively decouples the cross‐talk effects, thus breaking the infinite loop of side reactions. As a result, the Zn//V2O5 cells using this modified hydrogel electrolyte demonstrate stable operation over 1,000 cycles, with a capacity loss rate of only 0.028 % per cycle. Our study provides a promising gel chemistry, which offers a valuable guide for the construction of high‐performance and multifunctional aqueous Zn‐ion batteries. [ABSTRACT FROM AUTHOR]

The Zn//V2O5 system not only faces the incontrollable growth of zinc (Zn) dendrites, but also withstands the cross‐talk effect of by‐products produced from the cathode side to the Zn anode, inducing interelectrode talk and aggravating battery failure. To tackle these issues, we construct a rapid Zn2+‐conducting hydrogel electrolyte (R‐ZSO) to achieve Zn deposition modulation and side reaction inhibition in Zn//V2O5 full cells. The polymer matrix and BN exhibit a robust anchoring effect on SO42−, accelerating Zn2+ migration and enabling dense Zn deposition behavior. Therefore, the Zn//Zn symmetric cells based on the R‐ZSO electrolyte can operate stably for more than 1500 h, which is six times higher than that of cells employing the blank electrolyte. More importantly, the R‐ZSO hydrogel electrolyte effectively decouples the cross‐talk effects, thus breaking the infinite loop of side reactions. As a result, the Zn//V2O5 cells using this modified hydrogel electrolyte demonstrate stable operation over 1,000 cycles, with a capacity loss rate of only 0.028 % per cycle. Our study provides a promising gel chemistry, which offers a valuable guide for the construction of high‐performance and multifunctional aqueous Zn‐ion batteries. [ABSTRACT FROM AUTHOR]