A new apparatus was designed with a thick-walled glass capillary, electric heater tube with red copper and heat preservation. The thick-walled glass capillary was used for its advantages of resistance to acid corrosio...A new apparatus was designed with a thick-walled glass capillary, electric heater tube with red copper and heat preservation. The thick-walled glass capillary was used for its advantages of resistance to acid corrosion and pressure, and ease of observation. The experimental densities over the entire range of mole fraction for the binary mixture of p-xylene＋acetic acid and o-xylene＋acetic acid were measured using the new apparatus at temperatures ranging from 313.15K to 473.15K and pressure ranging from 0.20 to 2,0 MPa. The density values were used in the determination of excess molar volumes, W. The Redlich-Kister equation was used to fit the excess molar volume values, and the coefficients and estimate ot the standard error values were presented. The experimental resuits prove that the density measurement apparatus is successful.展开更多
We succeeded in designing an effective catalyst, V2O5-P2O5-K2O/Al2O3. SiO2, by which a high yield of PA,105wt% can be gained in middle-sized industrial fluidized bed apparatus without addition of any promoting gas.The...We succeeded in designing an effective catalyst, V2O5-P2O5-K2O/Al2O3. SiO2, by which a high yield of PA,105wt% can be gained in middle-sized industrial fluidized bed apparatus without addition of any promoting gas.The mechanisms of effects of P2O5, K2O and Al2O3 on the surface properties of V2O5 were investigated by means of TPD and XRD. And the selectivity of oxidation are explained.Addition of a great deal of P2O5 restrains the activity of donating surface oxygen from V2O5, but increases the number of sites which donate surface oxygen. Addition of K2O promotes donation of surface oxygen from V2O6, and decreases the number of sites of donating oxygen, on the other hand, addition of K|O makes the surface structure of V2O5 catalysts more stable. Coating a small amount of Al2O2 onto support, SiO2, restrains the activity of donating oxygen and increases the number of sites of donating surface oxygen from V2O5.展开更多
In this study, the adsorption of o-xylene was investigated using modified halloysite adsorbents. The modification of the halloysite adsorbents depended on thermal processing, treated sulphuric acid（Vl） and sodium hy...In this study, the adsorption of o-xylene was investigated using modified halloysite adsorbents. The modification of the halloysite adsorbents depended on thermal processing, treated sulphuric acid（Vl） and sodium hydroxide, water solution of ammonium chloride as well as hexadecylotrimethyloammonium bromide. Adsorption rate constants of the pseudo-second order models were compared for experiment carried in the batch system. Langmuir and Freundlich to fit the adsorption equilibrium experimental data. pseudo-first and models were able展开更多
The studies are conducted in laboratory to determine the adsorption-desorption behavior of BTX (benzene, toluene and o-xylene) in gas phase on Fe, Fe-Al pillared clays adsorbents. In experimental conditions of constan...The studies are conducted in laboratory to determine the adsorption-desorption behavior of BTX (benzene, toluene and o-xylene) in gas phase on Fe, Fe-Al pillared clays adsorbents. In experimental conditions of constant atmospheric pressure, initial concentrations with an increasing volume (0.5 - 2 ml) injected benzene (2.25), toluene (1.89) and o-xylene (1.66) μmol/L at T (40℃, 60℃ and 80℃), and the adsorption increases with increase of temperature, indicating that the adsorption process would be a chemical adsorption rather than physical one. The results are shown that the BTX adsorption data fitted very well (R2 > 0.999) to the both equations Langmuire and Elovitch for the three samples: bentonite (B), Fe-bentonite () and Fe-Al/bentonite (). At 80℃, the BTX adsorption capacity increased in the following order: . The maximum adsorption capacity () at 80℃ is 175.13, 171.84 and 171.81 μg/g respectively for benzene, toluene and o-xylene for;the last is a good adsorbent of BTX removal. The benzene diffuses faster than toluene and o-xylene. Thermodynamic parameters, such as ,and are also discussed and the results suggested that the BTX adsorption on all samples used is a spontaneous and endothermic process. Desorption studies show that BTX is very easily desorbed with .展开更多
The effect of pretreatment on Pd/Al2O3 catalysts for the catalytic oxidation of o-xylene at low temperature was studied by changing the pretreatment and testing conditions. The fresh and pretreated Pd/Al2O3 catalysts ...The effect of pretreatment on Pd/Al2O3 catalysts for the catalytic oxidation of o-xylene at low temperature was studied by changing the pretreatment and testing conditions. The fresh and pretreated Pd/Al2O3 catalysts were characterized by transmission electron microscopy （TEM）, X-ray photoelectron spectroscopy （XPS） and X-ray diffraction （XRD）. The results showed that the pretreatment dramatically changed the Pd/PdO ratio and then significantly affected the Pd/Al2O3 activity; while the pretreatment had not much influence on Pd particle size. The Pd/Al2O3 pre-reduced at 300~C/400~C, which has fully reduced Pd species, showed the highest activity; while the fresh Pd/Al2O3, which has fully oxidized Pd species, presented the worst performance, indicating the Pd chemical state plays an important role in the catalytic activity for the o-xylene oxidation. It is concluded that metallic Pd is the active species on the Pd/Al2O3 catalyst for the catalytic oxidation of o-xylene at low temperature.展开更多
The activities of CeO2 nanocubes calcined at different temperatures were tested for catalytic oxidation of o-xylene. Using CeO2 nanocubes as catalysts, complete catalytic oxidation of o-xylene was achieved below 210℃...The activities of CeO2 nanocubes calcined at different temperatures were tested for catalytic oxidation of o-xylene. Using CeO2 nanocubes as catalysts, complete catalytic oxidation of o-xylene was achieved below 210℃. The CeO2 nanomaterials were characterized by means of BET, X-ray diffraction （XRD）, transmission electron microscopy （TEM）, and high-resolution transmission electron microscopy （HRTEM）. From the TEM images, all CeO2 nanocubes displayed cubic morphology irrespective of calcination temperature. The HRTEM images revealed that these nanocubes were enclosed by reactive {001} planes, which may contribute to the intrinsically catalytic property of o-xylene oxidation. The higher activity of CeO2 nanocubes calcined at 550℃ than those calcined at above 550℃ was attributed to their smaller crystallite size and larger surface area. The influences of reaction conditions were also studied, which found that a higher reaction temperature was necessary for complete catalytic oxidation of o-xylene at higher weight hourly space velocity （WHSV） and o-xylene concentration.展开更多
Ce_(x)Co_(y)Cuzoxide composite catalysts were prepared by using polyethylene glycol, citrate sol-gel method combined with PMMA template for the oxidation of o-xylene. The catalysts were characterized by the Xray diffr...Ce_(x)Co_(y)Cuzoxide composite catalysts were prepared by using polyethylene glycol, citrate sol-gel method combined with PMMA template for the oxidation of o-xylene. The catalysts were characterized by the Xray diffraction(XRD), H2-temperature programmed reduction(H2-TPR), X-ray photoelectron spectroscopy(XPS) and Fourier transform infrared spectroscopy(FT-IR), etc. The catalytic activity for o-xylene was investigated. The catalytic degradation pathway and mechanism of o-xylene were inferred. The results show that Ce O_(2)is mainly present on the surface of all catalysts. The surface area of Ce_(2)Co1Cu1is up to 77.2 m^(2)/g, and the average pore size is 10.62 nm. It exhibits redox and sufficient Ce^(4+)and Ce^(^(3+)), and reactive oxygen species, and has maximum O-H and C=O in the five catalyst samples. The catalytic activity of Ce2Co1Cu1is the best at low temperature, with the T50and T90values of 235 and 258°C at a space velocity of 32000 h-1, respectively. The o-xylene is oxidized to o-methyl benzaldehyde, and then further oxidized to o-methylbenzoic acid, and finally CO_(2)and H2O are formed.展开更多
Pd/Al_(2)O_(3)was pretreated by CO,H_(2)and NaBH_(4)reduction,respectively.The reduced catalysts were tested for o-xylene oxidation and characterized by power X-ray diffraction(XRD),transmission electron microscopy (T...Pd/Al_(2)O_(3)was pretreated by CO,H_(2)and NaBH_(4)reduction,respectively.The reduced catalysts were tested for o-xylene oxidation and characterized by power X-ray diffraction(XRD),transmission electron microscopy (TEM),X-ray photoelectron spectroscopy (XPS) and temperature-programmed decomposition of palladium hydride (TPDH).The characterizations indicate the pretreatments lead to distinct Pd particle sizes and amount of surface activated oxygen species,which are responsible for the catalytic performance.Compared with H_(2)and NaBH_(4)reduction methods,CO reduction shows a strong interaction between Pd and Al_(2)O_(3)with smaller Pd particle size and more surface activated oxygen.It exhibited excellent catalytic performance,complete oxidation of 50 ppmV o-xylene at 85℃with a WHSV of 60,000 mL/(g·hr).展开更多
This paper reports fast and efficient chemical decontamination of water within a tree-branched centimeter-scale microfluidic reactor.The microreactor integrates Zinc oxide nanowires(ZnO NWs)in situ grown acting as an ...This paper reports fast and efficient chemical decontamination of water within a tree-branched centimeter-scale microfluidic reactor.The microreactor integrates Zinc oxide nanowires(ZnO NWs)in situ grown acting as an efficient photocatalytic nanomaterial layer.Direct growth of ZnO NWs within the microfluidic chamber brings this photocatalytic medium at the very close vicinity of the water flow path,hence minimizing the required interaction time to produce efficient purification performance.We demonstrate a degradation efficiency of 95%in o5 s of residence time in one-pass only.According to our estimates,it becomes attainable using microfluidic reactors to produce decontamination of merely 1 l of water per day,typical of the human daily drinking water needs.To conduct our experiments,we have chosen a laboratory-scale case study as a seed for addressing the health concern of water contamination by volatile organic compounds(VOCs),which remain difficult to remove using alternative decontamination techniques,especially those involving water evaporation.The contaminated water sample contains mixture of five pollutants:Benzene;Toluene;Ethylbenzene;m–p Xylenes;and o-Xylene(BTEX)diluted in water at 10 p.p.m.concentration of each.Degradation was analytically monitored in a selective manner until it falls below 1 p.p.m.for each of the five pollutants,corresponding to the maximum contaminant level(MCL)established by the US Environmental Protection Agency(EPA).We also report on a preliminary study,investigating the nature of the chemical by-products after the photocatalytic VOCs degradation process.展开更多
基金Supported by China Petrochemical Corporation(X505012)
文摘A new apparatus was designed with a thick-walled glass capillary, electric heater tube with red copper and heat preservation. The thick-walled glass capillary was used for its advantages of resistance to acid corrosion and pressure, and ease of observation. The experimental densities over the entire range of mole fraction for the binary mixture of p-xylene＋acetic acid and o-xylene＋acetic acid were measured using the new apparatus at temperatures ranging from 313.15K to 473.15K and pressure ranging from 0.20 to 2,0 MPa. The density values were used in the determination of excess molar volumes, W. The Redlich-Kister equation was used to fit the excess molar volume values, and the coefficients and estimate ot the standard error values were presented. The experimental resuits prove that the density measurement apparatus is successful.
文摘We succeeded in designing an effective catalyst, V2O5-P2O5-K2O/Al2O3. SiO2, by which a high yield of PA,105wt% can be gained in middle-sized industrial fluidized bed apparatus without addition of any promoting gas.The mechanisms of effects of P2O5, K2O and Al2O3 on the surface properties of V2O5 were investigated by means of TPD and XRD. And the selectivity of oxidation are explained.Addition of a great deal of P2O5 restrains the activity of donating surface oxygen from V2O5, but increases the number of sites which donate surface oxygen. Addition of K2O promotes donation of surface oxygen from V2O6, and decreases the number of sites of donating oxygen, on the other hand, addition of K|O makes the surface structure of V2O5 catalysts more stable. Coating a small amount of Al2O2 onto support, SiO2, restrains the activity of donating oxygen and increases the number of sites of donating surface oxygen from V2O5.
文摘In this study, the adsorption of o-xylene was investigated using modified halloysite adsorbents. The modification of the halloysite adsorbents depended on thermal processing, treated sulphuric acid（Vl） and sodium hydroxide, water solution of ammonium chloride as well as hexadecylotrimethyloammonium bromide. Adsorption rate constants of the pseudo-second order models were compared for experiment carried in the batch system. Langmuir and Freundlich to fit the adsorption equilibrium experimental data. pseudo-first and models were able
文摘The studies are conducted in laboratory to determine the adsorption-desorption behavior of BTX (benzene, toluene and o-xylene) in gas phase on Fe, Fe-Al pillared clays adsorbents. In experimental conditions of constant atmospheric pressure, initial concentrations with an increasing volume (0.5 - 2 ml) injected benzene (2.25), toluene (1.89) and o-xylene (1.66) μmol/L at T (40℃, 60℃ and 80℃), and the adsorption increases with increase of temperature, indicating that the adsorption process would be a chemical adsorption rather than physical one. The results are shown that the BTX adsorption data fitted very well (R2 > 0.999) to the both equations Langmuire and Elovitch for the three samples: bentonite (B), Fe-bentonite () and Fe-Al/bentonite (). At 80℃, the BTX adsorption capacity increased in the following order: . The maximum adsorption capacity () at 80℃ is 175.13, 171.84 and 171.81 μg/g respectively for benzene, toluene and o-xylene for;the last is a good adsorbent of BTX removal. The benzene diffuses faster than toluene and o-xylene. Thermodynamic parameters, such as ,and are also discussed and the results suggested that the BTX adsorption on all samples used is a spontaneous and endothermic process. Desorption studies show that BTX is very easily desorbed with .
基金supported by the Ministry of Science and Technology of China (No. 2012AA062702,2010AA64905)the National Natural Science Foundation of China (No. 21077117)
文摘The effect of pretreatment on Pd/Al2O3 catalysts for the catalytic oxidation of o-xylene at low temperature was studied by changing the pretreatment and testing conditions. The fresh and pretreated Pd/Al2O3 catalysts were characterized by transmission electron microscopy （TEM）, X-ray photoelectron spectroscopy （XPS） and X-ray diffraction （XRD）. The results showed that the pretreatment dramatically changed the Pd/PdO ratio and then significantly affected the Pd/Al2O3 activity; while the pretreatment had not much influence on Pd particle size. The Pd/Al2O3 pre-reduced at 300~C/400~C, which has fully reduced Pd species, showed the highest activity; while the fresh Pd/Al2O3, which has fully oxidized Pd species, presented the worst performance, indicating the Pd chemical state plays an important role in the catalytic activity for the o-xylene oxidation. It is concluded that metallic Pd is the active species on the Pd/Al2O3 catalyst for the catalytic oxidation of o-xylene at low temperature.
基金supported by the National Natural Science Foundation of China (No.50921064,20973193)the Ministry of Science and Technology of China (No.2007AA061402,2010CB732304)
文摘The activities of CeO2 nanocubes calcined at different temperatures were tested for catalytic oxidation of o-xylene. Using CeO2 nanocubes as catalysts, complete catalytic oxidation of o-xylene was achieved below 210℃. The CeO2 nanomaterials were characterized by means of BET, X-ray diffraction （XRD）, transmission electron microscopy （TEM）, and high-resolution transmission electron microscopy （HRTEM）. From the TEM images, all CeO2 nanocubes displayed cubic morphology irrespective of calcination temperature. The HRTEM images revealed that these nanocubes were enclosed by reactive {001} planes, which may contribute to the intrinsically catalytic property of o-xylene oxidation. The higher activity of CeO2 nanocubes calcined at 550℃ than those calcined at above 550℃ was attributed to their smaller crystallite size and larger surface area. The influences of reaction conditions were also studied, which found that a higher reaction temperature was necessary for complete catalytic oxidation of o-xylene at higher weight hourly space velocity （WHSV） and o-xylene concentration.
基金Project supported by the Zhejiang Provincial Natural Science Foundation of China (LY20E080003)。
文摘Ce_(x)Co_(y)Cuzoxide composite catalysts were prepared by using polyethylene glycol, citrate sol-gel method combined with PMMA template for the oxidation of o-xylene. The catalysts were characterized by the Xray diffraction(XRD), H2-temperature programmed reduction(H2-TPR), X-ray photoelectron spectroscopy(XPS) and Fourier transform infrared spectroscopy(FT-IR), etc. The catalytic activity for o-xylene was investigated. The catalytic degradation pathway and mechanism of o-xylene were inferred. The results show that Ce O_(2)is mainly present on the surface of all catalysts. The surface area of Ce_(2)Co1Cu1is up to 77.2 m^(2)/g, and the average pore size is 10.62 nm. It exhibits redox and sufficient Ce^(4+)and Ce^(^(3+)), and reactive oxygen species, and has maximum O-H and C=O in the five catalyst samples. The catalytic activity of Ce2Co1Cu1is the best at low temperature, with the T50and T90values of 235 and 258°C at a space velocity of 32000 h-1, respectively. The o-xylene is oxidized to o-methyl benzaldehyde, and then further oxidized to o-methylbenzoic acid, and finally CO_(2)and H2O are formed.
基金supported by the National Natural Science Foundation of China (Nos. 21936005 and 21806011)。
文摘Pd/Al_(2)O_(3)was pretreated by CO,H_(2)and NaBH_(4)reduction,respectively.The reduced catalysts were tested for o-xylene oxidation and characterized by power X-ray diffraction(XRD),transmission electron microscopy (TEM),X-ray photoelectron spectroscopy (XPS) and temperature-programmed decomposition of palladium hydride (TPDH).The characterizations indicate the pretreatments lead to distinct Pd particle sizes and amount of surface activated oxygen species,which are responsible for the catalytic performance.Compared with H_(2)and NaBH_(4)reduction methods,CO reduction shows a strong interaction between Pd and Al_(2)O_(3)with smaller Pd particle size and more surface activated oxygen.It exhibited excellent catalytic performance,complete oxidation of 50 ppmV o-xylene at 85℃with a WHSV of 60,000 mL/(g·hr).
基金This work has received funding from the ANR EquipEx SENSECITY projectthe FUI 18 MIMESYS funded by Region Ile-de-France and the European Union’s H2020 Programme for research,technological development and demonstration under grant agreement No 644852.
文摘This paper reports fast and efficient chemical decontamination of water within a tree-branched centimeter-scale microfluidic reactor.The microreactor integrates Zinc oxide nanowires(ZnO NWs)in situ grown acting as an efficient photocatalytic nanomaterial layer.Direct growth of ZnO NWs within the microfluidic chamber brings this photocatalytic medium at the very close vicinity of the water flow path,hence minimizing the required interaction time to produce efficient purification performance.We demonstrate a degradation efficiency of 95%in o5 s of residence time in one-pass only.According to our estimates,it becomes attainable using microfluidic reactors to produce decontamination of merely 1 l of water per day,typical of the human daily drinking water needs.To conduct our experiments,we have chosen a laboratory-scale case study as a seed for addressing the health concern of water contamination by volatile organic compounds(VOCs),which remain difficult to remove using alternative decontamination techniques,especially those involving water evaporation.The contaminated water sample contains mixture of five pollutants:Benzene;Toluene;Ethylbenzene;m–p Xylenes;and o-Xylene(BTEX)diluted in water at 10 p.p.m.concentration of each.Degradation was analytically monitored in a selective manner until it falls below 1 p.p.m.for each of the five pollutants,corresponding to the maximum contaminant level(MCL)established by the US Environmental Protection Agency(EPA).We also report on a preliminary study,investigating the nature of the chemical by-products after the photocatalytic VOCs degradation process.
