期刊
MATERIALS TODAY CHEMISTRY
卷 5, 期 -, 页码 52-62出版社
ELSEVIER SCI LTD
DOI: 10.1016/j.mtchem.2017.07.002
关键词
Mechanochemical; Ball-milling; Composites; One-pot oxidation; Hydrocarboxylation; Cyclohexane
资金
- Fundacao para a Ciencia e a Tecnologia, Portugal [SFRH/BPD/90883/2012, SFRH/BPD/108338/2015, IF/01270/2013/CP1163/CT0007, UID/QUI/00100/2013, PTDC/QEQ-QIN/3967/2014, UID/NAN/50024/2013]
- Instituto Politecnico de Lisboa (MechSynCat Project-Concurso Anual de IDICA) [710044/2016]
- Fundação para a Ciência e a Tecnologia [UID/NAN/50024/2013, PTDC/QEQ-QIN/3967/2014, IF/01270/2013/CP1163/CT0007] Funding Source: FCT
A simple and clean mechanochemical synthesis at room temperature was employed to prepare CuO-Fe2O3-CoCl2 (100 nm scale), MoO3-V2O5, CuO-CoCl2, Fe2O3-CoCl2, CuO-V2O5, Cu(CH3COO)(2)-V2O5, Cu(CH3COO)(2)-MoO3 (1-100 mm scale) 3d metal based dispersed composites with different ratios of components using simple metal salts/oxides and multiwalled carbon nanotubes (CNT) or graphene oxide (GO) additives (CoCl2-CNT, CoCl2-GO). The thus prepared composite materials were characterized by Xray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), field emission gun scanning electron microscopy (FEGSEM), energy-dispersive X-ray spectroscopy (EDX) and transmission electron microscopy (TEM). XPS analysis revealed no metal redox change upon ball milling treatment, which however promotes metal hydroxylation. The catalytic activity of the prepared composites in the heterogeneous low power microwave-assisted oxidation of cyclohexane with aq. H2O2 at 30 degrees C was notorious with yields up to 31% and selectivity up to 94% towards cyclohexanol (upon treatment with PPh3) for the CuO-CoCl2-based material. The hydro-carboxylation of cyclohexane with CO, water and K2S2O8 to produce cyclohexanecarboxylic acid bearing one more carbon atom at 60 degrees C is achieved with yields up to 17% for the reaction performed in the presence of the CuO-CoCl2 catalyst. The clean CuO-CoCl2 (1:2) catalyst preparation and the catalytic reaction (oxidation of cyclohexane) can be achieved in one-pot at low temperature, without any added organic solvent, and by using exclusively the mechanochemical energy input, with a marked 23% yield at 30 degrees C. (C) 2017 Elsevier Ltd. All rights reserved.
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