Ti/BMMs (Ti supported bimodal mesoporous silica) catalysts have been prepared via self-assembly route com- bined with ship-in-a-bottle method. The recovery and recycling performances of Ti/BMMs were investigated in ...Ti/BMMs (Ti supported bimodal mesoporous silica) catalysts have been prepared via self-assembly route com- bined with ship-in-a-bottle method. The recovery and recycling performances of Ti/BMMs were investigated in the epoxidation of cyclohexene. In order to the evaluate the regeneration methods and to examine the deactivation behaviors, the deactivated Ti/BMMs catalysts were washed in chloroform or calcinated at 450 ℃ for 6 h and then activity of the recovery catalysts were examined. Meanwhile, the structure features and surface properties of the regenerated catalysts were characterized by X-ray diffraction, N2-sorption analysis, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, thermogravi- metric analysis, UV visible spectroscopy and X-ray photoelectron spectroscopy. The results showed that the typical bimodal mesoporous structure of recycled Ti/BMMs catalysts was still maintained, and the phenomenon of Ti leaching during the catalytic process and recovery was negligible. In particular, spectroscopic observations indicated that the effects of the regeneration methods on the tetrahedrally-coordinated Ti species and catalytic deactivation were remarkable. The main reasons were related to the polarities of used solvents during recovery tests, the environment medium of adsorbed water inside mesopore channels and the deposition of bulky mole- cules of by-products on the mesoporous surface.展开更多
The degradation of 4-chloro-3-methylphenol(PCMC)using zeolite-encapsulated iron(III),nickel(II),and copper(II)complexes of N,N’-disalicylidene-1,2-phenylenediamine as catalysts,in a heterogeneous Fenton-like ...The degradation of 4-chloro-3-methylphenol(PCMC)using zeolite-encapsulated iron(III),nickel(II),and copper(II)complexes of N,N’-disalicylidene-1,2-phenylenediamine as catalysts,in a heterogeneous Fenton-like advanced oxidation process,was studied.The physicochemical properties of the catalysts were determined using powder X-ray diffraction,thermogravimetric analysis,Brunauer–Emmett–Teller surface area analysis,Fourier-transform infrared spectroscopy,elemental analysis,and scanning electron microscopy.The effects of four factors,namely initial H2O2 concentration,catalyst dosage,temperature,and pH,on the degradation of a model organic pollutant were determined.The results show that at low acidic pH,almost complete removal of PCMC was achieved with the iron(III),nickel(II),and copper(II)catalysts after 120 min under the optimum reaction conditions:catalyst dosage 0.1 g,H2O2 concentration 75 mmol/L,initial PCMC concentration 0.35mmol/L,and 50 °C.The reusability of the prepared catalysts in PCMC degradation was also studied and a possible catalyst deactivation mechanism is proposed.The possible intermediate products,degradation pathway,and kinetics of PCMC oxidation were also studied.展开更多
基金Supported by the National Natural Science Foundation of China(21076003,21272005)the Funding Project for the Academic Human Resources Development in Institutions of Higher Learning under the Jurisdiction of the Beijing Municipality(PHR201107104,005000541211019/20,005000543111517)
文摘Ti/BMMs (Ti supported bimodal mesoporous silica) catalysts have been prepared via self-assembly route com- bined with ship-in-a-bottle method. The recovery and recycling performances of Ti/BMMs were investigated in the epoxidation of cyclohexene. In order to the evaluate the regeneration methods and to examine the deactivation behaviors, the deactivated Ti/BMMs catalysts were washed in chloroform or calcinated at 450 ℃ for 6 h and then activity of the recovery catalysts were examined. Meanwhile, the structure features and surface properties of the regenerated catalysts were characterized by X-ray diffraction, N2-sorption analysis, scanning electron microscopy, transmission electron microscopy, Fourier transform infrared spectroscopy, thermogravi- metric analysis, UV visible spectroscopy and X-ray photoelectron spectroscopy. The results showed that the typical bimodal mesoporous structure of recycled Ti/BMMs catalysts was still maintained, and the phenomenon of Ti leaching during the catalytic process and recovery was negligible. In particular, spectroscopic observations indicated that the effects of the regeneration methods on the tetrahedrally-coordinated Ti species and catalytic deactivation were remarkable. The main reasons were related to the polarities of used solvents during recovery tests, the environment medium of adsorbed water inside mesopore channels and the deposition of bulky mole- cules of by-products on the mesoporous surface.
基金Leather Industry Development Institute(LIDI),Government of Ethiopia,Addis Ababa,for full financial support for his PhD studies under Twinning Program between Leather Industry Development Institute(LIDI),Addis Ababa University(AAU)and CSIR-Central Leather Research Institute(CLRI)
文摘The degradation of 4-chloro-3-methylphenol(PCMC)using zeolite-encapsulated iron(III),nickel(II),and copper(II)complexes of N,N’-disalicylidene-1,2-phenylenediamine as catalysts,in a heterogeneous Fenton-like advanced oxidation process,was studied.The physicochemical properties of the catalysts were determined using powder X-ray diffraction,thermogravimetric analysis,Brunauer–Emmett–Teller surface area analysis,Fourier-transform infrared spectroscopy,elemental analysis,and scanning electron microscopy.The effects of four factors,namely initial H2O2 concentration,catalyst dosage,temperature,and pH,on the degradation of a model organic pollutant were determined.The results show that at low acidic pH,almost complete removal of PCMC was achieved with the iron(III),nickel(II),and copper(II)catalysts after 120 min under the optimum reaction conditions:catalyst dosage 0.1 g,H2O2 concentration 75 mmol/L,initial PCMC concentration 0.35mmol/L,and 50 °C.The reusability of the prepared catalysts in PCMC degradation was also studied and a possible catalyst deactivation mechanism is proposed.The possible intermediate products,degradation pathway,and kinetics of PCMC oxidation were also studied.