Fe(III)-Based Phenylsilsesquioxane/Acetylacetonate Complexes: Synthesis, Cage-like Structure, and High Catalytic Activity

Alexey N. Bilyachenko, Victor N. Khrustalev, Pavel V. Dorovatovskii, Lidia S. Shul’pina, Nikolay S. Ikonnikov, Elena S. Shubina, Nikolai N. Lobanov, Vusala A. Aliyeva, Ana V. M. Nunes, Kamran T. Mahmudov, Yuriy N. Kozlov, Armando J. L. Pombeiro

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Abstract

Unprecedented iron-based silsesquioxane/acetylacetonate complexes were synthesized. The intriguing cage-like structure of compounds is alkaline metal-dependent: the Fe2Li2 complex includes condensed Si6-silsesquioxane and four acetylacetonate ligands; the Fe4Na4 complex exhibits two cyclic Si4-silsesquioxane and eight acetylacetonate ligands, while the Fe3K3 complex features two cyclic Si3-silsesquioxane and six acetylacetonate ligands. The latter case is the very first observation of small trimeric silsesquioxane ligands in the composition of cage-like metallasilsesquioxanes. The Fe4Na4-based complex exhibits a record high activity in the oxidation of inert alkanes with peroxides (55% yield of oxygenates in cyclohexane oxidation). It also acts as a catalyst in the cycloaddition of CO2 with epoxides, leading to cyclic carbonates in good yields (58-96%).
Original languageEnglish
Pages (from-to)1909-1918
Number of pages10
JournalInorganic Chemistry
Volume63
Issue number4
Early online date12 Jan 2024
DOIs
Publication statusPublished - 29 Jan 2024

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