Electrostatic effects drive graphene oxide carbon dots to self-assemble into negatively charged layer for constructing anti-aging zinc-ion batteries.

Hydrogen evolution reaction, corrosion, and zinc dendrite growth are the main bottlenecks limiting the performance of zinc-ion batteries. Additives are considered a direct and effective solution by adsorbing on the zinc anode surface to construct a protective layer. However, while traditional protective layers can suppress side reactions and corrosion, their non-uniform thickness and high interfacial impedance reduce the migration rate of Zn, leading to uneven Zn concentration distribution and actually exacerbating dendrite growth. Herein, graphene oxide carbon dots (GO-CDs) with multiple adsorption sites were designed. GO-CDs adsorb on the zinc anode surface through multiple sites and self-assemble to form a uniformly distributed multifunctional negatively charged layer. This negatively charged layer creates a water-deficient environment, effectively suppressing the hydrogen evolution reaction; electrostatically repels SO to avoid the formation of basic zinc sulfate corrosion products; and reconstructs the distribution of interfacial electric fields, establishing directional electrostatically driven mass transfer channels, enhancing the Zn migration rate, reducing the desolvation activation energy barrier, optimizing the nucleation overpotential, and achieving a spatially uniform distribution of Zn concentration, thereby inhibiting the growth of zinc dendrites. Performance tests show that Zn||Zn symmetric cells can maintain cycling stability for over 1800 h. Even after aging tests, restarted Zn||Zn symmetric cells can still maintain stable performance, with restarted Zn||Cu half-cells achieving a coulombic efficiency of up to 99.8%, in stark contrast to the failure of the control group.