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Catalytic hydrogenation rate of polycyclic aromatic hydrocarbons in supercritical carbon dioxide containing polymer-stabilized palladium nanoparticles |
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| Authors: | Liao Weisheng Liu Hsin-Wang Chen Hsing-Jung Chang Wen-Yen Chiu Kong-Hwa Wai Chien M |
| Institution: | a Department of Chemistry, University of Idaho, Moscow, ID 83844, USA b Department of Applied Science, National Dong Hwa University, Hualien 970, Taiwan, ROC c Department of Biomedical Engineering and Environmental Sciences, National Tsing Hua University, Hsinchu 300, Taiwan, ROC d Department of Chemistry, National Chung-Hsing University, Taichung 402, Taiwan, ROC e Department of Natural Sciences, National Science Council, Taipei 107, Taiwan, ROC |
| Abstract: | Catalytic hydrogenation of polycyclic aromatic hydrocarbons (PAHs) with up to four fused benzene rings over high-density-polyethylene-stabilized palladium nanoparticles in supercritical carbon dioxide via in situ UV/Vis spectroscopy is presented. PAHs can be efficiently converted to saturated polycyclic hydrocarbons using this green technique under mild conditions at 20 MPa of CO2 containing 1 MPa of H2 at 40-50 °C. Kinetic studies based on in situ UV/Vis spectra of the CO2 phase reveal that the initial hydrogenation of a given PAH and the subsequent hydrogenations of its intermediates are pseudo-first-order. The hydrogenation rate of the latter is always much smaller than that of the former probably due to increasing steric hindrance introduced by the hydrogenated benzene rings of PAHs which impedes the adsorption process and hydrogen access to PAHs on catalyst surfaces. |
| Keywords: | PAHs Supercritical carbon dioxide Catalytic hydrogenation Palladium nanoparticles |
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