Tuning the structure of fe-tetracarboxylate frameworks through linker-symmetry reduction

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Abstract

The design and synthesis of stable metal–organic frameworks (MOFs) have been a core obstacle in the widespread application of these functional crystalline porous materials, because of the stability limitations of MOFs under harsh operating conditions. Herein, a highly stable microporous MOF based on the Fe3O cluster (PCN-678) has been synthesized using a tetracarboxylate ligand. Utilizing symmetry reduced tetratopic carboxylate ligand, a mesoporous MOF (PCN-668) could be obtained in which nanoscale cage-like building units and one-dimensional (1D) channels coexist. The neighboring cages were mutual diastereomers in PCN-668 due to the further reduction of the Cs symmetry of the free ligand to C1 symmetry after self-assembly. Furthermore, the acid stability of this mesoporous MOF was improved via postsynthetic metal exchange to chromium (PCN-668-Cr). The PCN-668-Cr exhibited very high stability in both acidic and basic aqueous solutions (pH = 1–11). Additionally, the mesoporous MOF showed a high total gravimetric methane uptake (∼500 cm3 g−1 at 100 bar), while the microporous MOF showed a high volumetric methane storage capacity of 147 cm3 cm−3 at room temperature.

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Pang, J., Lollar, C. T., Che, S., Qin, J. S., Li, J., Cai, P., … Zhou, H. C. (2021). Tuning the structure of fe-tetracarboxylate frameworks through linker-symmetry reduction. CCS Chemistry, 3(2), 1701–1709. https://doi.org/10.31635/ccschem.020.202000348

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