This article briefly reviewed the advances in the process of the direct oxidation of methane to methanol (DMTM) with both heterogeneous and homogeneous oxidation. Attention was paid to the conversion of methane by t...This article briefly reviewed the advances in the process of the direct oxidation of methane to methanol (DMTM) with both heterogeneous and homogeneous oxidation. Attention was paid to the conversion of methane by the heterogeneous oxidation process with various transition metal ox‐ides. The most widely studied catalysts are based on molybdenum and iron. For the homogeneous gas phase oxidation, several process control parameters were discussed. Reactor design has the most crucial role in determining its commercialization. Compared to the above two systems, aque‐ous homogenous oxidation is an efficient route to get a higher yield of methanol. However, the cor‐rosive medium in this method and its serious environmental pollution hinder its widespread use. The key challenge to the industrial application is to find a green medium and highly efficient cata‐lysts.展开更多
This paper represents the interaction of well characterized Lewis base [(Pyr)nCuX]4O2, n = 1 or 2, X = Cl, Br or I, Pyr = pyrrolidine with CO2 as a Lewis acid to produce new series of oxidative coupling and catechol...This paper represents the interaction of well characterized Lewis base [(Pyr)nCuX]4O2, n = 1 or 2, X = Cl, Br or I, Pyr = pyrrolidine with CO2 as a Lewis acid to produce new series of oxidative coupling and catechol oxidase initiators [(Pyr)nCuX]4(CO3)2. These carbonato derivatives are isolated as stable solids. They are easily soluble in aprotic solvents as CH2Cl2 or PhNO2. Cryoscopic measurements support tetranuclear core structure for all of them. Infrared spectra show differences from their oxo analogous in the carbonato domains but those differences did not distinguish between tridentate bridging carbonato and bidentate one. Rate of oxidation of 2,6-dimethylphenol (DMP) by [(Pyr)CuCl]4(CO3)2, supports coordination number six for Cu(Ⅱ) centers in [(Pyr)CuCl]4(CO3)2. In order to fulfill coordination number six, for n = 1, carbonate will act as tridentate while for n = 2, it will act as bidentate, as shown in Scheme 4. Near infrared spectra indicate a [(3 halo) Cu(Ⅱ) charge transfer] for [(Pyr)nCuX]4(CO3)2, n = 1 or 2, X = Cl or Br. Low molecular absorptivities of the maxima at 825 nm and 730 nm for [(Pyr)nCuI]4(CO3)2, n = 1 or 2 with a minimum of high molecular absorptivities at 600 nm, comparing to X= CI or Br analogous, support a step structure for [(Pyr),Cul]4(CO3)2, as shown in Scheme 5. Cyclic voltammograms for [(Pyr)nCuX]4(CO3)2; n = 1 or 2, X = CI or Br, are irreversible in characters.展开更多
The sulfurous water deposit exploitation in volcanic, swamp, or wetland regions, represents an alternative option for potable water supply in cities and communities around the world. However, before its consumption, i...The sulfurous water deposit exploitation in volcanic, swamp, or wetland regions, represents an alternative option for potable water supply in cities and communities around the world. However, before its consumption, it must be treated by the application of physicochemical or biological methods with the ability to separate high contents in sulfates, hydrogen sulphite and sulphides which have laxative, allergic and toxic properties in humans. Conventional methods require the supply of chemical compounds or the adequate control of different parameters such as pH, temperature, etc., and the constant maintenance within their reactors. For these reasons, the systems could have elevated operating costs and require additional steps to enable the treatment of its separated products and the final disposal of its residual waste generated. In this research, compound parabolic collectors are implemented for the use of solar energy radiation, UV-B type, in Solar Advanced Oxidation Processes in H2O2/O3/UVsolar homogeneous phase. Its application during the pre-treatment of four sulfur water wells from the region of Puebla, Mexico, demonstrated its ability to transform their sulfur compounds in sulfates of easy removal by a later stage of reverse osmosis, in an approximately 15 min treatment time process.展开更多
CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction(SCR) of NOx with NH3 were p...CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction(SCR) of NOx with NH3 were prepared by an incipient-wetness impregnation method. These catalysts were characterized by means of BET, XRD, UV–Vis,Raman and XPS techniques. The results showed that the catalytic activity of V2O5–WO3/TiO2 was greatly enhanced by Ce doping(molar ratio of Ce/Ti = 1/10) in the TiO2 support.The catalysts that were predominantly anatase TiO2 showed better catalytic performance than the catalysts that were predominantly fluorite CeO2. The Ce additive could enhance the surface adsorbed oxygen and accelerate the SCR reaction. The effects of O2 concentration, ratio of NH3/NO, space velocity and SO2 on the catalytic activity were also investigated. The presence of oxygen played an important role in NO reduction. The optimal ratio of NH3/NO was 1/1 and the catalyst had good resistance to SO2 poisoning.展开更多
基金supported by the Petrochemical Joint Funds of NSFC-CNPC (U1362202)the Postgraduate Innovation Project of China University of Petroleum (East China) (YCXJ2016030)~~
文摘This article briefly reviewed the advances in the process of the direct oxidation of methane to methanol (DMTM) with both heterogeneous and homogeneous oxidation. Attention was paid to the conversion of methane by the heterogeneous oxidation process with various transition metal ox‐ides. The most widely studied catalysts are based on molybdenum and iron. For the homogeneous gas phase oxidation, several process control parameters were discussed. Reactor design has the most crucial role in determining its commercialization. Compared to the above two systems, aque‐ous homogenous oxidation is an efficient route to get a higher yield of methanol. However, the cor‐rosive medium in this method and its serious environmental pollution hinder its widespread use. The key challenge to the industrial application is to find a green medium and highly efficient cata‐lysts.
文摘This paper represents the interaction of well characterized Lewis base [(Pyr)nCuX]4O2, n = 1 or 2, X = Cl, Br or I, Pyr = pyrrolidine with CO2 as a Lewis acid to produce new series of oxidative coupling and catechol oxidase initiators [(Pyr)nCuX]4(CO3)2. These carbonato derivatives are isolated as stable solids. They are easily soluble in aprotic solvents as CH2Cl2 or PhNO2. Cryoscopic measurements support tetranuclear core structure for all of them. Infrared spectra show differences from their oxo analogous in the carbonato domains but those differences did not distinguish between tridentate bridging carbonato and bidentate one. Rate of oxidation of 2,6-dimethylphenol (DMP) by [(Pyr)CuCl]4(CO3)2, supports coordination number six for Cu(Ⅱ) centers in [(Pyr)CuCl]4(CO3)2. In order to fulfill coordination number six, for n = 1, carbonate will act as tridentate while for n = 2, it will act as bidentate, as shown in Scheme 4. Near infrared spectra indicate a [(3 halo) Cu(Ⅱ) charge transfer] for [(Pyr)nCuX]4(CO3)2, n = 1 or 2, X = Cl or Br. Low molecular absorptivities of the maxima at 825 nm and 730 nm for [(Pyr)nCuI]4(CO3)2, n = 1 or 2 with a minimum of high molecular absorptivities at 600 nm, comparing to X= CI or Br analogous, support a step structure for [(Pyr),Cul]4(CO3)2, as shown in Scheme 5. Cyclic voltammograms for [(Pyr)nCuX]4(CO3)2; n = 1 or 2, X = CI or Br, are irreversible in characters.
文摘The sulfurous water deposit exploitation in volcanic, swamp, or wetland regions, represents an alternative option for potable water supply in cities and communities around the world. However, before its consumption, it must be treated by the application of physicochemical or biological methods with the ability to separate high contents in sulfates, hydrogen sulphite and sulphides which have laxative, allergic and toxic properties in humans. Conventional methods require the supply of chemical compounds or the adequate control of different parameters such as pH, temperature, etc., and the constant maintenance within their reactors. For these reasons, the systems could have elevated operating costs and require additional steps to enable the treatment of its separated products and the final disposal of its residual waste generated. In this research, compound parabolic collectors are implemented for the use of solar energy radiation, UV-B type, in Solar Advanced Oxidation Processes in H2O2/O3/UVsolar homogeneous phase. Its application during the pre-treatment of four sulfur water wells from the region of Puebla, Mexico, demonstrated its ability to transform their sulfur compounds in sulfates of easy removal by a later stage of reverse osmosis, in an approximately 15 min treatment time process.
基金financially supported by the National Natural Science Foundation of China (Nos. 21376261, 21173270, 21177160)the National Hi-Tech Research and Development Program (863) of China (No. 2013AA065302)+2 种基金the Beijing Natural Science Foundation (2142027)the Doctoral Selection Fund (No. 20130007110007)the China University of Petroleum Fund (No. KYJJ2012-06-31)
文摘CeO2–TiO2composite supports with different Ce/Ti molar ratios were prepared by a homogeneous precipitation method, and V2O5–WO3/CeO2–TiO2catalysts for the selective catalytic reduction(SCR) of NOx with NH3 were prepared by an incipient-wetness impregnation method. These catalysts were characterized by means of BET, XRD, UV–Vis,Raman and XPS techniques. The results showed that the catalytic activity of V2O5–WO3/TiO2 was greatly enhanced by Ce doping(molar ratio of Ce/Ti = 1/10) in the TiO2 support.The catalysts that were predominantly anatase TiO2 showed better catalytic performance than the catalysts that were predominantly fluorite CeO2. The Ce additive could enhance the surface adsorbed oxygen and accelerate the SCR reaction. The effects of O2 concentration, ratio of NH3/NO, space velocity and SO2 on the catalytic activity were also investigated. The presence of oxygen played an important role in NO reduction. The optimal ratio of NH3/NO was 1/1 and the catalyst had good resistance to SO2 poisoning.