Electrochemical catalysis of styrene epoxidation with films of MnO 2 nanoparticles and H2O2

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作者
Espinal, Laura [1 ,3 ]
Suib, Steven L. [1 ,2 ,3 ]
Rusling, James F. [1 ,3 ,4 ]
机构
[1] Department of Chemistry, University of Connecticut, Storrs, CT 06269-3060, United States
[2] Department of Chemical Engineering, University of Connecticut, Storrs, CT 06269-3060, United States
[3] Institute of Materials Sciences, University of Connecticut, Storrs, CT 06269-3060, United States
[4] Department of Pharmacology, Univ. of Connecticut Health Center, Farmington, CT 06032, United States
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Catalysis - Electrochemistry - Hydrogen peroxide - Manganese compounds - Nanostructured materials;
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摘要
Films of polyions and octahedral layered manganese oxide (OL-1) nanoparticles on carbon electrodes made by layer-by-layer alternate electrostatic adsorption were active for electrochemical catalysis of styrene epoxidation in solution in the presence of hydrogen peroxide and oxygen. The highest catalytic turnover was obtained by using applied voltage -0.6 V vs SCE, O2, and 100 mM H2O2. 18O isotope labeling experiments suggested oxygen incorporation from three different sources: molecular oxygen, hydrogen peroxide, and/or lattice oxygen from OL-1 depending on the potential applied and the oxygen and hydrogen peroxide concentrations. Oxygen and hydrogen peroxide activate the OL-1 catalyst for the epoxidation. The pathway for styrene epoxidation in the highest yields required oxygen, hydrogen peroxide, and a reducing voltage and may involve an activated oxygen species in the OL-1 matrix.
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页码:7676 / 7682
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