With the rapid growth of renewable energy sources such as wind and solar power, the demand for large-scale, cost-effective, and safe energy storage systems has received tremendous attention recently. Among these, aqueous zinc-ion batteries (AZIBs) have emerged as a promising candidate for grid-scale energy storage due to their high volumetric energy density, intrinsic safety, and abundant availability of Zn sources. However, the commercial viability of AZIBs is currently severely hindered by the poor reversibility of the Zn metal anode. In aqueous electrolytes, the Zn anode suffers from uncontrolled dendrite growth caused by non-uniform ion flux as well as parasitic side reactions like hydrogen evolution and corrosion induced by the activity of free water molecules. These coupled degradation processes continuously consume the limited aqueous electrolyte and generate insulating byproducts, inevitably leading to battery swelling, rapid capacity decay, and premature cell failure. Traditional protection strategies such as electrolyte additives and passive interfacial coatings often struggle to simultaneously achieve the homogenization of ion flux and the precise regulation of solvation structures, leading to a trade-off between interfacial stability and ionic conductivity. To address these critical challenges, ion-sieving frameworks including zeolites, metal-organic frameworks (MOFs), and covalent organic frameworks (COFs) have attracted significant attention. Unlike conventional passive barriers, these materials possess sub-nano to nano-scale regular channels that can effectively regulate ionic transport behavior at the molecular level. This review systematically summarizes the latest advances in utilizing ion-sieving frameworks for high-performance Zn anode protection. First, we elucidate the fundamental microscopic mechanisms of ion sieving. Specifically, the sub-nanometer pores of these frameworks physically confine hydrated Zn ions and force them to shed their solvation sheaths, thereby separating active water molecules from the electrode surface and suppressing their side reactions. This critical desolvation process drastically alters the coordination environment, lowering the activation energy barrier for subsequent charge transfer kinetics. Concurrently, the ordered channel arrays rectify the chaotic ion flux into uniform streams, eliminating local concentration gradients and inhibiting dendrite nucleation during prolonged plating and stripping cycles. Furthermore, through electrostatic repulsion or size exclusion, the frameworks facilitate selective ion transport by effectively blocking harmful anions and polysulfides while allowing the rapid migration of Zn ions. Subsequently, the structure-property relationships of three typical framework materials are analyzed. Inorganic zeolites are highlighted for their rigid pores and high thermal stability, making them ideal for physical sieving; MOFs offer tunable pore environments and quasi-solid-state transport channels enriched with versatile metal nodes; while COFs are noted for their lightweight skeletons and precise functional group customization, allowing for the targeted design of highly conductive ion-hopping sites. The application strategies of these materials are then categorized into three levels: constructing artificial solid electrolyte interphase (ASEI) layers for direct surface protection, developing functionalized separators to intercept crosstalk between electrodes, and formulating solid-state/quasi-solid-state electrolytes to achieve intrinsic safety. This review also comprehensively discusses the remaining challenges and future perspectives of this field. The need for advanced in-situ characterization techniques coupled with theoretical computations to unravel the dynamic ion transport mechanisms within the confined channels is strongly emphasized. Furthermore, to bridge the gap between laboratory research and practical application, future efforts must focus on developing scalable, cost-effective, and ultrathin membrane fabrication technologies. Importantly, evaluating these framework-modified anodes under stringent, commercially relevant conditions—such as low negative-to-positive (N/P) capacity ratios, lean electrolyte volumes, and high areal capacities—is crucial for their eventual deployment. We conclude that the evolution from liquid-state to solid-state systems, enabled by ion-sieving frameworks, represents a vital pathway towards the development of next-generation AZIBs with long cycle life and high energy density.
Liu et al. (Sun,) studied this question.