| Title |
Nucleation Rate Governs Crystal Quality in 100 g-Scale Aqueous Synthesis of ZIF-Based MOFs for Semi-Solid-State Lithium Metal Batteries |
| Authors |
(Jiwoo Yoon) ; (Sangbaek Park) |
| DOI |
https://doi.org/10.3365/KJMM.2026.64.10.896 |
| ISSN |
1738-8228(ISSN), 2288-8241(eISSN) |
| Keywords |
Metal-organic frameworks; Aqueous synthesis; Large-batch synthesis; Semi-solid-state electrolytes; Lithium metal batteries |
| Abstract |
Metal-organic frameworks (MOFs) are promising hosts for semi-solid-state electrolytes (SSSEs) because their ordered micropores can confine liquid electrolyte while providing regulated pathways for Li-ion transport. However, producing such MOFs uniformly and with high crystallinity in large quantities remains challenging, particularly through aqueous routes that avoid the solvent-handling burden associated with organic synthesis. Herein, we report that the crystal quality of zeolitic imidazolate framework-8 (ZIF-8) in 100 g-scale aqueous synthesis is governed by the nucleation rate: a long precursor feeding time slows nucleation and produces heterogeneous particles with poorly developed crystallinity, whereas a short feeding time consistently promotes rapid nucleation and uniform, well-defined polyhedral particles. Similarly, a Cu/Zn bimetallic MOF yields uniformly faceted crystals, indicating that this nucleation-growth criterion is transferable across compositions. The resulting ZIF-8 and Cu/Zn MOFs successfully retain their microporous structures with surface areas comparable to those of laboratory-scale ZIF-based MOFs, and remain intact while effectively hosting electrolyte within their pores after separator fabrication. These separators exhibit ionic conductivities typical of MOF-based SSSEs, a wider anodic stability window than a commercial separator with liquid electrolyte, stable long-term Li plating/stripping, and high capacity retention in Li || LiFePO4 (LFP) cells. These results demonstrate that the nucleation rate is key to maintaining MOF quality during large-scale aqueous synthesis without sacrificing the characteristics required for SSSE applications |