The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed...The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed that the Ni/TiO2-SiO2 catalyst calcined at 700 ℃ had high and stable activity while the catalysts calcined at 550 and 850 ℃ had low and unstable activity. Depending on the calcination temperature, one, two, or three of the following Ni-containing species, NiO, Ni2.44Ti0.72Si0.07O4, and NiTiO3 were identified by combining the temperature programmed reduction (TPR) and X-ray diffraction (XRD) results. Their reducibility decreased in the sequence: NiO〉Ni2.44Ti0.72Si0.07O4〉NiTiO3. It suggests that high and stable activities observed over the Ni/TiO2-SiO2 catalyst calcined at 700 ~C were induced by the formation of Ni2.44Ti0.72Si0.07O4 and smaller NiO species crystallite size.展开更多
采用正交实验初步确定了Ni P SiO2/TiO2纳米化学复合镀工艺的基本配方。研究了搅拌速度、表面活性剂加入量、pH值、温度对沉积速度的影响,以及纳米粒子加入量、搅拌方式、搅拌速度、表面活性剂种类对镀层纳米粒子复合量的影响,得出最... 采用正交实验初步确定了Ni P SiO2/TiO2纳米化学复合镀工艺的基本配方。研究了搅拌速度、表面活性剂加入量、pH值、温度对沉积速度的影响,以及纳米粒子加入量、搅拌方式、搅拌速度、表面活性剂种类对镀层纳米粒子复合量的影响,得出最佳工艺配方。展开更多
Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by...Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support.展开更多
According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equatio...According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equation for photocatalysis of Procion Red MX-5B was built.Response surface and contour were graphed with the decoloration rate of Procion Red MX-5B as the response value.Based on the analysis of the response surface plots and their corresponding contour plots,effects of pH value,irradiation time and catalyst loading were explored.By using this new method,the optimum decoloration condition was obtained as follows:pH value,1.3;irradiation time,49.9 min;catalyst loading,0.57 g/L.In the optimization,R-Squared and Adj R-Squared correlation coefficients for quadratic model were evaluated quite satisfactorily as 0.9310 and 0.8620,respectively.Under the optimum conditions established,the performance of 99.47% for color removal was experimentally reached.It was found that all factors considered have an important effect on the decolorization efficiency of Procion Red MX-5B.By the ANOVA analysis and model confirmation the optimal solution obtained using RSM was experimentally validated and credible with preferable instructional ability for experiments.展开更多
In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including...In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including feedstock gases space velocity,coke content,bed temperature and sulfur-tolerant stability of 100 h life were investigated.The structure of the catalysts was characterized by XRD,N2adsorptiondesorption and TEM.It is found that under same space velocity from 5000 h 1to 25000 h 1FBR gave a higher CH4yield,lower coke content,and lower bed temperature than those obtained in FIXBR.Ni-W/TiO2-SiO2catalyst possessed excellent sulfur-tolerant stability on the feedstock gases less than 500 ppm H2S in FBR.The carbon deposits formed on the spent catalyst were in the form of carbon fibers in FBR,while in the form of dense accumulation distribution appearance in FIXBR.展开更多
A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic re...A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic reduction(SCR) performance and SO2-resistant ability of TiO2-SiO2-WO3 were greatly enhanced by the introduction of cerium. The catalyst containing 10% CeO2 showed the highest NO conversion in a wide temperature range and good N2 selectivity with broad operation temperature window at the gas hourly space velocity(GHSV) of 30000 h–1, which was a very promising catalyst for NOx abatement from diesel engine exhaust. The catalysts were characterized by X-ray diffraction(XRD), scanning electron microscopy with energy dispersive X-ray spectroscopy(SEM-EDS), N2 adsorption-desorption(BET) and X-ray photoelectron spectroscopy(XPS). The characterization results showed that the bigger pore radius, higher surface atomic concentration and dispersion of Ce and the abundant adsorbed oxygen on the surface of catalyst contributed to the best NH3-SCR performance of CeO2/TiO2-SiO2-WO3 catalyst containing 10% CeO2.展开更多
A series of SO 2- 4/TiO 2 SiO 2 catalysts with different mass fractions of SiO 2 were prepared by sol gel method. The effect of adding SiO 2 on the crystal structure, specific surface area, oxygen adsorption, and acid...A series of SO 2- 4/TiO 2 SiO 2 catalysts with different mass fractions of SiO 2 were prepared by sol gel method. The effect of adding SiO 2 on the crystal structure, specific surface area, oxygen adsorption, and acidity of SO 2- 4/TiO 2 catalyst and its photocatalytic property for degradation of bromomethane was studied. The results showed that the specific surface area and amount of oxygen adsorption of catalyst were increased by addition of SiO 2, leading to the obvious increase on photocatalytic activity of SO 2- 4/TiO 2 SiO 2 catalysts and mineralization ratio of bromomethane. Comparing with SO 2- 4/TiO 2, the acidic strength and anti moisture ability of SO 2- 4/TiO 2 SiO 2 catalyst were decreased.展开更多
The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over Ni/TiO2 catalysts prepared by a liquid-phase chemical reduction method. The catalysts were characterized by inductively coupled plasm...The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over Ni/TiO2 catalysts prepared by a liquid-phase chemical reduction method. The catalysts were characterized by inductively coupled plasma (ICP), X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS) and temperature-programmed reduction (TPR). Results show that the titania structure has favorable influence on physio-chemical and catalytic properties of Ni/TiO2 catalysts. Compared to commercial Raney nickel, the catalytic activity of Ni/TiO2 catalyst is much superior, irrespective of the titania structure. The catalytic activity of anatase titania supported nickel catalyst Ni/TiO2(A) is higher than that of rutile titania supported nickel catalyst Ni/TiO2(R), possibly because the reduction of nickel oxide to metallic nickel for Ni/TiO2(A) is easier than that for Ni/TiO2(R) at similar reaction conditions.展开更多
摘要The influence of calcination temperature on the structure and catalytic behavior of Ni/TiO2-SiO2 catalyst, for CO2 reforming of methane to synthesis gas under atmospheric pressure, was investigated. The results showed that the Ni/TiO2-SiO2 catalyst calcined at 700 ℃ had high and stable activity while the catalysts calcined at 550 and 850 ℃ had low and unstable activity. Depending on the calcination temperature, one, two, or three of the following Ni-containing species, NiO, Ni2.44Ti0.72Si0.07O4, and NiTiO3 were identified by combining the temperature programmed reduction (TPR) and X-ray diffraction (XRD) results. Their reducibility decreased in the sequence: NiO〉Ni2.44Ti0.72Si0.07O4〉NiTiO3. It suggests that high and stable activities observed over the Ni/TiO2-SiO2 catalyst calcined at 700 ~C were induced by the formation of Ni2.44Ti0.72Si0.07O4 and smaller NiO species crystallite size.
基金Financial support from the National Natural Science Foundation of China (21163019) is gratefully acknowledged
摘要Ni/Al_2O_3-SiO_2 catalysts were synthesized via one-step method employing SiO_2 as an additive for the selective hydrogenation of butyne-1,4-diol(B_3D) to butane-1,4-diol(B1D). The prepared catalysts were evaluated by a series of characterization techniques including BET, XRD, SEM, EDX-mapping, TEM, H_2-TPR, XPS, NH_3-TPD and Py-FTIR. Compared to Ni/Al_2O_3 catalyst, the SiO_2-doped samples exhibited better B_3D conversion. SiO_2 could help to form a strong interaction between NiO with the support, which inhibited Ni agglomeration at high temperature, improved the Ni dispersion, and enhanced the hydrogenation activity. B_1D selectivity was mainly influenced by the quantity of Lewis acid sites in addition to the Ni dispersion. The catalyst with a silica loading of 6.4% demonstrated an excellent selectivity of 75.18%(by 13% higher than the contrastive Ni/Al_2O_3 catalyst), which was attributed to the larger amount of Lewis acid sites and the moderate interaction between NiO with the support, which could facilitate the nickel dispersion on a preferable surface area of 176.3 m^2/g of support.
基金Sponsored by the National Natural Science Foundation of China (Grant No. 51078100)the National Creative Research Groups granted by NSFC(Grant No. 50821002)+1 种基金Excellent Youth Foundation of Heilongjiang Scientific Committee(Grant No. JC2010-03)State Key Laboratory of Urban Water Resource and Environment(Grant No. 2010DX11)
摘要According to the design principle of the central composite experimental,the method of response surface analysis with three factors and three levels was adopted based on one factor test.A second-order quadratic equation for photocatalysis of Procion Red MX-5B was built.Response surface and contour were graphed with the decoloration rate of Procion Red MX-5B as the response value.Based on the analysis of the response surface plots and their corresponding contour plots,effects of pH value,irradiation time and catalyst loading were explored.By using this new method,the optimum decoloration condition was obtained as follows:pH value,1.3;irradiation time,49.9 min;catalyst loading,0.57 g/L.In the optimization,R-Squared and Adj R-Squared correlation coefficients for quadratic model were evaluated quite satisfactorily as 0.9310 and 0.8620,respectively.Under the optimum conditions established,the performance of 99.47% for color removal was experimentally reached.It was found that all factors considered have an important effect on the decolorization efficiency of Procion Red MX-5B.By the ANOVA analysis and model confirmation the optimal solution obtained using RSM was experimentally validated and credible with preferable instructional ability for experiments.
摘要In this work,syngas methanation over Ni-W/TiO2-SiO2catalyst was studied in a fluidized-bed reactor(FBR)and its performance was compared with a fixed-bed reactor(FIXBR).The effects of main operating variables including feedstock gases space velocity,coke content,bed temperature and sulfur-tolerant stability of 100 h life were investigated.The structure of the catalysts was characterized by XRD,N2adsorptiondesorption and TEM.It is found that under same space velocity from 5000 h 1to 25000 h 1FBR gave a higher CH4yield,lower coke content,and lower bed temperature than those obtained in FIXBR.Ni-W/TiO2-SiO2catalyst possessed excellent sulfur-tolerant stability on the feedstock gases less than 500 ppm H2S in FBR.The carbon deposits formed on the spent catalyst were in the form of carbon fibers in FBR,while in the form of dense accumulation distribution appearance in FIXBR.
基金supported by the National Natural Science Foundation of China(21173153)the National High Technology Research and Development Program of China(863 project)(2013AA065304)
摘要A series of catalysts were prepared by doping different loadings of CeO2 over TiO2-SiO2-WO3 and used for the selective catalytic reduction of NOx by NH3. The experimental results showed that the selective catalytic reduction(SCR) performance and SO2-resistant ability of TiO2-SiO2-WO3 were greatly enhanced by the introduction of cerium. The catalyst containing 10% CeO2 showed the highest NO conversion in a wide temperature range and good N2 selectivity with broad operation temperature window at the gas hourly space velocity(GHSV) of 30000 h–1, which was a very promising catalyst for NOx abatement from diesel engine exhaust. The catalysts were characterized by X-ray diffraction(XRD), scanning electron microscopy with energy dispersive X-ray spectroscopy(SEM-EDS), N2 adsorption-desorption(BET) and X-ray photoelectron spectroscopy(XPS). The characterization results showed that the bigger pore radius, higher surface atomic concentration and dispersion of Ce and the abundant adsorbed oxygen on the surface of catalyst contributed to the best NH3-SCR performance of CeO2/TiO2-SiO2-WO3 catalyst containing 10% CeO2.
摘要A series of SO 2- 4/TiO 2 SiO 2 catalysts with different mass fractions of SiO 2 were prepared by sol gel method. The effect of adding SiO 2 on the crystal structure, specific surface area, oxygen adsorption, and acidity of SO 2- 4/TiO 2 catalyst and its photocatalytic property for degradation of bromomethane was studied. The results showed that the specific surface area and amount of oxygen adsorption of catalyst were increased by addition of SiO 2, leading to the obvious increase on photocatalytic activity of SO 2- 4/TiO 2 SiO 2 catalysts and mineralization ratio of bromomethane. Comparing with SO 2- 4/TiO 2, the acidic strength and anti moisture ability of SO 2- 4/TiO 2 SiO 2 catalyst were decreased.
基金Supported by the National Basic Research Program (No.2003CB615702) and the National Natural Science Foundation of Chin(No.20436030).
摘要The catalytic hydrogenation of p-nitrophenol to p-aminophenol was investigated over Ni/TiO2 catalysts prepared by a liquid-phase chemical reduction method. The catalysts were characterized by inductively coupled plasma (ICP), X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectra (XPS) and temperature-programmed reduction (TPR). Results show that the titania structure has favorable influence on physio-chemical and catalytic properties of Ni/TiO2 catalysts. Compared to commercial Raney nickel, the catalytic activity of Ni/TiO2 catalyst is much superior, irrespective of the titania structure. The catalytic activity of anatase titania supported nickel catalyst Ni/TiO2(A) is higher than that of rutile titania supported nickel catalyst Ni/TiO2(R), possibly because the reduction of nickel oxide to metallic nickel for Ni/TiO2(A) is easier than that for Ni/TiO2(R) at similar reaction conditions.