Aqueous zinc-ion batteries (AZIBs) have garnered significant attention due to their inherent safety and cost-effectiveness, with electrolyte additives playing a pivotal role in enhancing their electrochemical performance. However, the current research landscape reveals a notable gap in the exploration of colloidal additives for AZIBs electrolyte systems. This study addresses this limitation by introducing a novel colloidal electrolyte system comprising two synergistic components: a dissolved fraction that modulates the Zn2+ solvation structure through small molecules, and an insoluble colloidal fraction that facilitates the formation of a robust solid-electrolyte interphase (SEI) at the anode surface. We propose the innovative use of perylene-3, 4, 9, 10-tetracarboxylic acid diimide (PTCDI) as a multifunctional colloidal additive to engineer a hybrid electrolyte with weak solvation effects. The PTCDI additive demonstrates unique multisite zincophilicity and hydrophobicity, effectively reducing free water content and nucleation potential within the hydrogen bonding network, thereby promoting uniform zinc nucleation. Moreover, PTCDI facilitates the formation of a novel solubilized structure during the desolvation process, enabling in situ generation of a stable SEI through water molecule substitution and enhanced anionic access to the solvation shell. This innovative approach yields remarkable electrochemical performance, achieving stable zinc stripping/plating for 2800 hours with a minimal overpotential of 58.4 mV and an exceptional Coulombic efficiency of 99.94%. Our findings establish colloidal additives as a promising paradigm for advancing AZIBs electrolyte design, offering new insights into the development of high-performance zinc-ion battery systems.
