Dynamic structural and morphological transformations in high-entropy metal-organic frameworks

High-entropy metal-organic frameworks (HE-MOFs) offer a promising approach for advanced applications like energy storage, catalysis, and sensing, thanks to their high configurational entropy and synergistic effects from multiple elements. Despite the progress in synthesizing HE-MOFs, primarily through solvothermal methods, little is known about the reticular chemistry governing morphological variations. This work presents a new class of porphyrinic HE-MOFs, offering insights into the lattice transformations by controlling secondary building unit (SBU) topology. The study also explores spatial configuration and dynamic elemental composition, proposing that metal incorporation, spatial variation, and node stability are influenced by metal precursor dissociation and metal-oxygen bond strength, which dictate long-term structural dynamics. • Developed a new class of porphyrinic high-entropy metal-organic frameworks (HE-MOFs) with tunable secondary building unit (SBU) topology. • Elucidated the mechanism of dynamic structural and morphological transformations driven by metal precursor dissociation and metal–oxygen bond strength. • Demonstrated spatial and compositional heterogeneity in HE-MOFs, revealing pathways for tailoring long-term structural stability.