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Interplay between H-bonding and interpenetration in an aqueous copper(II)–aminoalcohol–pyromellitic acid system: self-assembly synthesis, structural features and catalysis

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Abstract

Two new copper(II) coordination compounds, [Cu(H1.5mdea)2]2(H2pma) (1a) and [{Cu2(μ-Hmdea)2}24-pma)]n·2nH2O (1b), were self-assembled at different temperatures from the same multicomponent reaction system, comprising copper(II) nitrate, N-methyldiethanolamine (H2mdea), pyromellitic acid (H4pma), and potassium hydroxide. Products 1a and 1b were isolated as microcrystalline solids and fully characterized and their structures were established by single-crystal X-ray diffraction. Compound 1a features the bis-aminoalcohol(ate) monocopper(II) units and H2pma2− anions that are multiply interconnected by strong H-bonds into a firm 2D H-bonded layer. Compound 1b reveals the bis-aminoalcoholate dicopper(II) motifs that are interlinked by the μ4-pma4− spacers into a 3D + 3D interpenetrated metal–organic framework. From a topological perspective, both networks of 1a and 1b are uninodal and driven by similar 4-connected H2pma2− or pma4− nodes, but result in distinct sql and dia topologies, respectively. Compound 1a was applied as an efficient catalyst for two model cycloalkane functionalization reactions: (1) oxidation by H2O2 to form cyclic alcohols and ketones and (2) hydrocarboxylation by CO/H2O and S2O82− to form cycloalkanecarboxylic acids. The substrate scope, effects of various reaction parameters, selectivity and mechanistic features were also investigated.

Graphical abstract: Interplay between H-bonding and interpenetration in an aqueous copper(ii)–aminoalcohol–pyromellitic acid system: self-assembly synthesis, structural features and catalysis

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Publication details

The article was received on 21 Jul 2018, accepted on 29 Oct 2018 and first published on 29 Oct 2018


Article type: Paper
DOI: 10.1039/C8DT02983K
Citation: Dalton Trans., 2018, Advance Article
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    Interplay between H-bonding and interpenetration in an aqueous copper(II)–aminoalcohol–pyromellitic acid system: self-assembly synthesis, structural features and catalysis

    T. A. Fernandes, M. V. Kirillova, V. André and A. M. Kirillov, Dalton Trans., 2018, Advance Article , DOI: 10.1039/C8DT02983K

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