Assembly of an iron-based complex into a metal-organic framework: a space confinement strategy for isolation of mono-iron complexes to protect from dimerization

Juan Chen, Lu Qi Bai, Yi Fei Dai, Li Cheng Deng, Yu Wang, Tao Zhang, Kai Jie Chen

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2 引用 (Scopus)

摘要

Non-heme mononuclear iron complexes, especially when supported by tripodal tetradentate ligands, show promising C-H bond activation efficiency in catalytic reactions. Nevertheless, they intrinsically decay readily to their dinuclear form, and the dimerization process is inevitable in homogenous solution, which dramatically hinders their further application. Hence, we demonstrate that the mononuclear iron complex [(TPA)FeII-2L]2+ (L = labile ligands, mainly solvent molecules) was successfully encapsulated in a highly robust metal-organic framework UiO-66 via a two-step “ship-in-a-bottle” strategy. The nearly perfect size matching of the octahedral cages of the host UiO-66 provides ideal space confinement for the guest complex to protect from dimerization and dramatically increases the mono-nuclear complex stability compared to its un-confined state. The successful encapsulation of [(TPA)FeII-2L]2+ in UiO-66 was verified thoroughly by spectroscopy, microscopy, N2 adsorption, and electrochemistry characterization techniques. This work shows that encapsulating an unstable molecular complex in MOFs via a two-step “ship-in-a-bottle” strategy highlights opportunities for extending the heterogenization of homogeneous complexes.

源语言英语
页(从-至)18053-18060
页数8
期刊Dalton Transactions
52
47
DOI
出版状态已出版 - 10 11月 2023

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