This ranearch is focused on the, develonment of a simnle design model of the submerged catalysis/membrane filtration （catalysis/MF） system for phenol hydroxylation over TS-1 based on the material balance of the phen...This ranearch is focused on the, develonment of a simnle design model of the submerged catalysis/membrane filtration （catalysis/MF） system for phenol hydroxylation over TS-1 based on the material balance of the phenol under steady state and the reported kinetic studies. Based on the developed model, the theoretical phenol Conversions at steady state could be calculated using the kinetic parameters obtained from the previous batch experiments. The theoretical conversions are in good agreement with the experimental data obtained in the submerged catalysis/MF system within relative error of ±5%. The model can be used to determine the optimal experimental conditions to carry out the phenol hydroxylation over TS-1 in the submerged catalysis/MF system.展开更多
The present work synthesizes La-Cu4FeAlCO3 catalyst under microwave irradiation and characterizes its structure using XRD and IR techniques. The results show that the obtained La-Cu4FeAlCO3 has a hydrotalcite structur...The present work synthesizes La-Cu4FeAlCO3 catalyst under microwave irradiation and characterizes its structure using XRD and IR techniques. The results show that the obtained La-Cu4FeAlCO3 has a hydrotalcite structure. In the phenol hydroxylation with H2O2 catalyzed by La-Cu4FeAlCO3, the effects of reaction time and phenol/H2O2 molar ratio on the phenol hy-droxylation, and relationships between the initial hydroxylation rate with concentration of the catalyst, phenol, H2O2 and reaction temperature are also investigated in details. It is shown the phenol conversion can reach 50.09% (mol percent) in the phenol hydroxylation catalyzed by La-Cu4FeAlCO3, under the reaction conditions of the molar ratio of phenol/H2O2 1/2, the amount ratio of phenol/catalyst 20, reaction temperature 343 K, reaction time 120 min, 10 mL distilled water as solvent. Moreover, a kinetic equation of v = k[La ? Cu 4 FeAlCO 3 ][C 6 H 5 OH][H 2 O 2]. and the activation energy of Ea=58.37 kJ/mol are obtained according to the kinetic studies. Due to the fact that the HO-Cu+-OH species are detected in La-Cu4FeAlCO3/H2O2 system by XPS, the new mechanism about the generation of hydroxyl free radicals in the phenol hydroxylation is pro-posed, which is supposed that HO-Cu+-OH species are transition state in this reaction.展开更多
A new type of non-soluble copper aluminophosphate（denoted as CuAlPO） was synthesized by（static） hydrothermal crystallization and characterized by using several physicochemical techniques.XRD analysis reveals that ...A new type of non-soluble copper aluminophosphate（denoted as CuAlPO） was synthesized by（static） hydrothermal crystallization and characterized by using several physicochemical techniques.XRD analysis reveals that CuAlPO can be obtained from a reactive gel of molar composition: iso-Pr2NH∶0.3CuO∶（0.7Al2O3∶）P2O5∶80H2O in a Teflon-lined stainless steel autoclave at 180 ℃ for 72 h and has the same crystal structure as that of hexagonal SiO2（JCPDS No.83-2299）.The sources of CuO,Al2O3 and P2O5 were copper sulfate pentahydrate,aluminum isopropoxide and o-phosphoric acid（mass fraction: 85%）,respectively.SEM shows a characteristic hexagonal morphology and a crystallite size of about 2 μm for both the as-synthesized CuAlPO and the calcined CuAlPO（550 ℃,6h）.Low specific surace area（2.0 m2/g） and pore volume（0.004 mL/g） of CuAlPO were observed by N2-adsorption measurement.Catalytic evaluation tests demonstrate that an excellent transformation of phenol into catechol and hydroquinone over the material was achieved in water under the benign reaction conditions with a phenol conversion of 29.5% being observed at room temperature（30 ℃）.展开更多
基金Supported by the National-Basic Research Program of China （2009CB623406）, the National High Technology Research and Development Program of China （2007AA06A402） and the National Natural Science Foundation of China （20636020）.
文摘This ranearch is focused on the, develonment of a simnle design model of the submerged catalysis/membrane filtration （catalysis/MF） system for phenol hydroxylation over TS-1 based on the material balance of the phenol under steady state and the reported kinetic studies. Based on the developed model, the theoretical phenol Conversions at steady state could be calculated using the kinetic parameters obtained from the previous batch experiments. The theoretical conversions are in good agreement with the experimental data obtained in the submerged catalysis/MF system within relative error of ±5%. The model can be used to determine the optimal experimental conditions to carry out the phenol hydroxylation over TS-1 in the submerged catalysis/MF system.
文摘The present work synthesizes La-Cu4FeAlCO3 catalyst under microwave irradiation and characterizes its structure using XRD and IR techniques. The results show that the obtained La-Cu4FeAlCO3 has a hydrotalcite structure. In the phenol hydroxylation with H2O2 catalyzed by La-Cu4FeAlCO3, the effects of reaction time and phenol/H2O2 molar ratio on the phenol hy-droxylation, and relationships between the initial hydroxylation rate with concentration of the catalyst, phenol, H2O2 and reaction temperature are also investigated in details. It is shown the phenol conversion can reach 50.09% (mol percent) in the phenol hydroxylation catalyzed by La-Cu4FeAlCO3, under the reaction conditions of the molar ratio of phenol/H2O2 1/2, the amount ratio of phenol/catalyst 20, reaction temperature 343 K, reaction time 120 min, 10 mL distilled water as solvent. Moreover, a kinetic equation of v = k[La ? Cu 4 FeAlCO 3 ][C 6 H 5 OH][H 2 O 2]. and the activation energy of Ea=58.37 kJ/mol are obtained according to the kinetic studies. Due to the fact that the HO-Cu+-OH species are detected in La-Cu4FeAlCO3/H2O2 system by XPS, the new mechanism about the generation of hydroxyl free radicals in the phenol hydroxylation is pro-posed, which is supposed that HO-Cu+-OH species are transition state in this reaction.
文摘A new type of non-soluble copper aluminophosphate（denoted as CuAlPO） was synthesized by（static） hydrothermal crystallization and characterized by using several physicochemical techniques.XRD analysis reveals that CuAlPO can be obtained from a reactive gel of molar composition: iso-Pr2NH∶0.3CuO∶（0.7Al2O3∶）P2O5∶80H2O in a Teflon-lined stainless steel autoclave at 180 ℃ for 72 h and has the same crystal structure as that of hexagonal SiO2（JCPDS No.83-2299）.The sources of CuO,Al2O3 and P2O5 were copper sulfate pentahydrate,aluminum isopropoxide and o-phosphoric acid（mass fraction: 85%）,respectively.SEM shows a characteristic hexagonal morphology and a crystallite size of about 2 μm for both the as-synthesized CuAlPO and the calcined CuAlPO（550 ℃,6h）.Low specific surace area（2.0 m2/g） and pore volume（0.004 mL/g） of CuAlPO were observed by N2-adsorption measurement.Catalytic evaluation tests demonstrate that an excellent transformation of phenol into catechol and hydroquinone over the material was achieved in water under the benign reaction conditions with a phenol conversion of 29.5% being observed at room temperature（30 ℃）.
