A series of novel catalysts consisting of nanosized Au particles confined in micro-mesoporous ZSM-5/SBA-15 （ZSBA） materials with platelet （PL）, rod （RD）, and hexagonal-prism （HP） morphologies have been synthes...A series of novel catalysts consisting of nanosized Au particles confined in micro-mesoporous ZSM-5/SBA-15 （ZSBA） materials with platelet （PL）, rod （RD）, and hexagonal-prism （HP） morphologies have been synthesized in situ. These catalysts possess both SBA-15 and ZSM-5 structures and exhibit excellent stability of their active sites by confinement of the Au nanoparticles （NPs） within ZSBA. The catalysts have been characterized in depth to understand their structure-property relationships. The gold NP dimensions and the pore structure of the catalysts, which were found to be sensitive to calcination temperature and synthetic conditions, are shown to play vital roles in the reduction of 4-nitrophenol. Au/ZSBA-PL, with short mesochannels （210 nm） and a large pore diameter （6.7 nm）, exhibits high catalytic performance in the reduction of 4-nitrophenol, whereas Au/ZSBA-HP and Au/ZSBA-RD, with long mesochannels and relatively smaller pore sizes, show poor catalytic activities. In the case of catalysts with different gold NP sizes, Au/ZSBA-PL-350 with an Au NP diameter of 4.0 nm exhibits the highest reaction rate constant （0.14 min-1） and turnover frequency （0.0341 s-1）. In addition, the effect of the reaction parameters on the reduction of 4-nitrophenol has been systematically investigated. A possible mechanism for 4-nitrophenol reduction over the Au/ZSBA catalysts is proposed.展开更多
基金This work was financially supported by the National Natural Science Foundation of China （Nos. 21573286, 21576288, and 21276277）, the Ministry of Science and Technology of China （Nos. 2011BAK15B05 and 2015AA034603）, the Specialized Research Fund for the Doctoral Program of Higher Education （No. 20130007110003）, Science Foundation of China Univer- sity of Petroleum, Beijing （No. 2462015YQ0304）.
文摘A series of novel catalysts consisting of nanosized Au particles confined in micro-mesoporous ZSM-5/SBA-15 （ZSBA） materials with platelet （PL）, rod （RD）, and hexagonal-prism （HP） morphologies have been synthesized in situ. These catalysts possess both SBA-15 and ZSM-5 structures and exhibit excellent stability of their active sites by confinement of the Au nanoparticles （NPs） within ZSBA. The catalysts have been characterized in depth to understand their structure-property relationships. The gold NP dimensions and the pore structure of the catalysts, which were found to be sensitive to calcination temperature and synthetic conditions, are shown to play vital roles in the reduction of 4-nitrophenol. Au/ZSBA-PL, with short mesochannels （210 nm） and a large pore diameter （6.7 nm）, exhibits high catalytic performance in the reduction of 4-nitrophenol, whereas Au/ZSBA-HP and Au/ZSBA-RD, with long mesochannels and relatively smaller pore sizes, show poor catalytic activities. In the case of catalysts with different gold NP sizes, Au/ZSBA-PL-350 with an Au NP diameter of 4.0 nm exhibits the highest reaction rate constant （0.14 min-1） and turnover frequency （0.0341 s-1）. In addition, the effect of the reaction parameters on the reduction of 4-nitrophenol has been systematically investigated. A possible mechanism for 4-nitrophenol reduction over the Au/ZSBA catalysts is proposed.
