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Issue 20, 2016
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Alkali α-MnO2/NaxMnO2 collaboratively catalyzed ammoxidation–Pinner tandem reaction of aldehydes

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Abstract

The tandem reaction is a growing field to yield important advances toward green and sustainable chemistry. Herein, we report a bifunctional manganese oxide catalyst with an interface binding redox phase (α-MnO2) and a basic phase (NaxMnO2). The molar ratio of NaOH/Mn plays a great role in the formation of α-MnO2/NaxMnO2. The sodium cation is essential for the formation of a basic NaxMnO2 phase while the potassium cation promotes the formation of a redox-active α-MnO2 phase. The interface structure of α-MnO2/NaxMnO2 geometrically favors the ammoxidation–Pinner tandem reaction to synthesize imidates in a 58–96% yield from aldehydes. Thus a phase collaborative effect is observed. In the ammoxidation process, the redox cycle of MnIV/MnIII is involved and the lattice oxygen in the α-MnO2 phase acts as an active oxygen species. The O–H in methanol is activated and dissociated on the basic sites of NaxMnO2 to the adsorbed methoxyl species to facilitate the Pinner synthesis. This approach bypasses the conventional synthesis of imidates, which suffer from harsh reaction conditions and the requirement for multiple steps.

Graphical abstract: Alkali α-MnO2/NaxMnO2 collaboratively catalyzed ammoxidation–Pinner tandem reaction of aldehydes

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Publication details

The article was received on 21 Apr 2016, accepted on 05 Aug 2016 and first published on 05 Aug 2016


Article type: Paper
DOI: 10.1039/C6CY00874G
Catal. Sci. Technol., 2016,6, 7429-7436

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    Alkali α-MnO2/NaxMnO2 collaboratively catalyzed ammoxidation–Pinner tandem reaction of aldehydes

    X. Jia, J. Ma, M. Wang, X. Li, J. Gao and J. Xu, Catal. Sci. Technol., 2016, 6, 7429
    DOI: 10.1039/C6CY00874G

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