An Ultrastable, Easily Scalable and Regenerable Macrocycle-Based Hydrogen-Bonded Organic Framework

Crystalline porous materials are increasingly significant in synthetic and materials chemistry. Nonetheless, their broad industrial deployment is hampered by challenges in stability, production cost, scalability, and regenerability. Herein, we introduce a one-pot synthetic methodology for fabricating macrocycle-based hydrogen-bonded organic frameworks utilizing commercially available materials. Notably, mHOF-SYSU101, as a distinguished exemplar, can be synthesized on a multigram scale with near-quantitative yield from raw materials of merely 70% purity, underscoring its substantial cost-efficiency. mHOF-SYSU101 demonstrates extraordinary thermal stability up to 400 °C, and exhibits remarkable chemical resilience under complex and harsh conditions over a week. This sustained stability is attributed to the strategic integration of hydrophobic methyl groups that insulate hydrogen bonds from polar molecules, coupled with multiple non-covalent interactions within its architecture. Leveraging its intrinsic one-dimensional hydrophobic channels and hydrophilic surfaces, mHOF-SYSU101 achieves a remarkable 99% adsorption of iodine from seawater in just 2 minutes and maintains this fully reversible adsorption capacity over five cycles, showing great practical utility for the nuclear power industry. Moreover, mHOF-SYSU101 can be regenerated by introducing its trifluoroacetic acid solution into dimethyl sulfoxide or methanol, endowing mHOF-SYSU101 with unprecedented processibility and recyclability. This study paves new pathways for achieving the industrial application of crystalline porous materials.

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