Electrochemical catalysis of styrene epoxidation with films of MnO2 nanoparticles and H2O2

被引:198
作者
Espinal, L
Suib, SL [1 ]
Rusling, JF
机构
[1] Univ Connecticut, Dept Chem, Storrs, CT 06269 USA
[2] Univ Connecticut, Dept Chem Engn, Storrs, CT 06269 USA
[3] Univ Connecticut, Inst Mat Sci, Storrs, CT 06269 USA
[4] Univ Connecticut, Ctr Hlth, Dept Pharmacol, Farmington, CT 06032 USA
关键词
D O I
10.1021/ja048940x
中图分类号
O6 [化学];
学科分类号
0703 ;
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, O(2), and 100 mM H(2)O(2). (18)O 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
页数:7
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