摘要
A versatile wet impregnation method was employed to conveniently and controllably deposit Fe_2O_3 nanoparticles on zeolites including commercial Y, mordenite and ZSM-5 with the similar framework Si/Al ratios and crystal sizes, respectively. The ultrafine Fe_2O_3 nanoparticles in size of 5 nm can be highly dispersed on zeolite Y matrix due to its much better wettability than ZSM-5 and mordenite. By using the obtained Fe_2O_3/zeolite composite as the heterogeneous Fenton-like catalysts, the degradation of phenol as a model reaction was systematically investigated, including the zeolite supports, particle size and dispersion of Fe_2O_3, and reaction conditions of H_2O_2 concentration, temperature, and pH value. The catalyst based on zeolite Y with Fe loading of 9% exhibited the best phenol degradation efficiency (> 90%)in neutral pH within 2 h. Its high catalytic activity in Fenton reaction can be attributed to the bifunctional properties of strong surface BrФnsted acidity and high reactivity of octahedral Fe^(3+) in the highlydispersed ultrafine Fe_2O_3 nanoparticles in size of 5 nm, which were the primary active centers to quickly decompose H_2O_2 into hydroxyl radicals. Since phenol degradation can be performed under mild conditions of ambient temperature (283-323 K) and a wide pH range (4.0-7.0), the catalysts can be easily recovered for recyclable use with stable degradation activity, which own the immense potential in deep treatment of organic pollutants in industrial wastewater.
A versatile wet impregnation method was employed to conveniently and controllably deposit Fe_2O_3 nanoparticles on zeolites including commercial Y, mordenite and ZSM-5 with the similar framework Si/Al ratios and crystal sizes, respectively. The ultrafine Fe_2O_3 nanoparticles in size of 5 nm can be highly dispersed on zeolite Y matrix due to its much better wettability than ZSM-5 and mordenite. By using the obtained Fe_2O_3/zeolite composite as the heterogeneous Fenton-like catalysts, the degradation of phenol as a model reaction was systematically investigated, including the zeolite supports, particle size and dispersion of Fe_2O_3, and reaction conditions of H_2O_2 concentration, temperature, and pH value. The catalyst based on zeolite Y with Fe loading of 9% exhibited the best phenol degradation efficiency (> 90%)in neutral pH within 2 h. Its high catalytic activity in Fenton reaction can be attributed to the bifunctional properties of strong surface BrФnsted acidity and high reactivity of octahedral Fe^(3+) in the highlydispersed ultrafine Fe_2O_3 nanoparticles in size of 5 nm, which were the primary active centers to quickly decompose H_2O_2 into hydroxyl radicals. Since phenol degradation can be performed under mild conditions of ambient temperature (283-323 K) and a wide pH range (4.0-7.0), the catalysts can be easily recovered for recyclable use with stable degradation activity, which own the immense potential in deep treatment of organic pollutants in industrial wastewater.
基金
sponsored by Shanghai Pujiang Program, China (No. 16PJ1401100)
the Shanghai Committee of Science and Technology, China (No.15ZR1402000)
Key Basic Research Program of Science and Technology Commission of Shanghai Municipality (No. 17JC1400100)
the NSF of China(No. 21673048)
National Youth Top Talent Support Program of National High-Level Personnel of Special Support Program (Youth Top-notch Talent Support Program)
the State Key Laboratory of Transducer Technology of China (No. SKT1503)
