Dendrite-free zinc anode enabled by bifunctional additive coupling electrostatic shielding and zincophilic leveling

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2024-01, Vol.480, p.148267, Article 148267
• Main Authors: Gong, Jingyao, Ying, Jinhui, Jia, Xiongjie, Su, Ruihang, Zhao, Tianshou, Jiang, Haoran
• Format: Article
• Language: English
• Subjects: Bifunctional effect; Electrolyte additive; Energy storage; Zinc dendrite; Zinc-based battery
• ISSN: 1385-8947
• DOI: 10.1016/j.cej.2023.148267

[Display omitted] •A novel bifunctional sodium citrate (Na3CA) electrolyte additive is proposed.•The citrate ion shows zincophilic leveling effect to reduce side reactions.•The sodium ion shows electrostatic shielding effect to inhibit zinc dendrites.•The symmetrical battery is stably cycled for more than 3500 h at 0.5 mA cm−2.•Na3CA leads to a substantial reduction in capacity decay after 500 cycles. The development of aqueous zinc-based batteries is hindered by the dendrite formation and side reactions. To address the issues, a novel bifunctional sodium citrate (Na3CA) electrolyte additive is developed, in which sodium ion forms an electrostatic shielding layer on the zinc surface to suppress the growth of zinc dendrites, while zincophilic citrate ion replaces water molecules in the solvent shell through leveling effect to reduce side reactions and adsorb onto the electrode surface to promote the uniform zinc deposition. Results show that in the symmetrical tests, the addition of Na3CA additive decreases the nucleation overpotential from 64.3 mV to 31.6 mV, enabling the battery to be stably cycled for more than 3500 h at the current density of 0.5 mA cm−2, which is 14 times higher than that with the traditional electrolyte. In the half-battery test, the Na3CA additive significantly improves the reversibility of the zinc anode with the average coulombic efficiency increasing from 87 % to 95 %. Full battery test shows that after 500 cycles, the capacity retention rate of the battery with Na3CA additive is 1.6 times that of the traditional battery. This work offers a facile and effective strategy of designing bifunctional electrolyte additive to achieve high-performance aqueous zinc-based batteries.