The understanding and controllable synthesis of mesoporous metal-organic frameworks (meso-MOFs) are attractive in various applications, especially in the case that involves large sized molecules. However, due to the contradiction and competition between the crystallization process of MOFs and the co-assembly of micelles with the building blocks of MOFs, the formation of single-crystal meso-MOFs with long-range ordered structure at both micro and mesoscopic scales is challenging. Herein, a strong and weak acids co-mediated cooperative assembly strategy is demonstrated to fabricate the single-crystal meso-MOFs nanoparticles with ordered meso-structure (p6mm), tunable mesopore size (6.1-40 nm) and particle size (45-750 nm). We demonstrate that the combination of strong inorganic and weak organic acids can precisely regulate the crystallization of MOFs and co-assembly behavior of micelles in the MOFs, directly resulting in the formation of meso-MOFs with both ordered mesopore channels and single crystalline frameworks. Importantly, based on this brand-new strategy, we constructed a library of unprecedented meso-MOFs with various morphology (cube, octahedron, 2D intersecting nanosheets, core-shells, hollow-shells and yolk-shells) and multivariate components (mixed functional ligands and metal ions). The resultant meso-MOFs greatly enhances corrosion resistance and prolonging the battery life in the application of aqueous zinc-ion batteries anodes by combining de-solvation and rapid zinc ion transfer process in the micropore and mesopore channels, respectively. We believe that this facile strategy opens up new horizons for synthesis of other mesoporous MOFs or other mesoporous single-crystal materials.

Strong and weak acids co-mediated cooperative assembly strategy for the synthesis of single-crystal meso-MOFs

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