分别通过自组装法(AS)和浸渍法(WI)制备得到纳米催化剂Pt/γ-Al2O3-AS和Pt/γ-Al2O3-WI,并用于评价甲苯、异丙醇、丙酮、乙酸乙酯等易挥发性有机物(VOCs)的氧化性能.通过各种表征手段探究了催化剂形态、结构及表面性质与催化剂氧化活性...分别通过自组装法(AS)和浸渍法(WI)制备得到纳米催化剂Pt/γ-Al2O3-AS和Pt/γ-Al2O3-WI,并用于评价甲苯、异丙醇、丙酮、乙酸乙酯等易挥发性有机物(VOCs)的氧化性能.通过各种表征手段探究了催化剂形态、结构及表面性质与催化剂氧化活性的关系.结果表明,Pt/γ-Al2O3-AS在低温下即可实现VOCs的完全氧化.在气体浓度(体积分数)为1000×10-6,空速为18000 m L·g-1·h-1的条件下,甲苯、异丙醇、丙酮、乙酸乙酯被Pt/γ-Al2O3-AS催化剂完全氧化的温度分别为130、135、145、215°C,展现出了优异的氧化性能,且具有很好的稳定性.该催化剂较高的比表面积、较小的Pt纳米粒径、较好的Pt纳米颗粒分散度、更好的低温还原效果及丰富的表面羟基是具有较高催化活性的重要因素.展开更多
Pt/BaO/Al_2O_3 catalysts with different BaO loadings prepared from Al_2O_3 nanorods(Pt/BaO/Al_2O_3-nr) and irregular Al_2O_3 nanoparticles(Pt/BaO/Al_2O_3-np) were investigated for NOx storage and reduction(NSR). The P...Pt/BaO/Al_2O_3 catalysts with different BaO loadings prepared from Al_2O_3 nanorods(Pt/BaO/Al_2O_3-nr) and irregular Al_2O_3 nanoparticles(Pt/BaO/Al_2O_3-np) were investigated for NOx storage and reduction(NSR). The Pt/BaO/Al_2O_3 materials derived from Al_2O_3 nanorods always exhibited much higher NOx storage capacity(NSC) over the whole temperature range of 100–400°C than the corresponding Pt/BaO/Al_2O_3-np samples containing the same BaO loading, giving the maximum NSC value of 966.9 μmol/gcatat 400°C, 1.4 times higher than that of Pt/BaO/Al_2O_3-np. Higher catalytic performance of nanorod-supported NSR samples was also observed during lean-rich cyclic conditions(90 sec vs. 5 sec), giving more than 98% NOx conversion at 300–450°C over the Pt/BaO/Al_2O_3-nr sample with 15% BaO loading. To reveal this dependence on the shape of the support during the NSR process, a series of characterization techniques including the Brunauer–Emmett–Teller(BET) method,X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), H_2 temperature programmed reduction(H2-TPR), and in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) were also conducted. It was found that intimate contact of Ba–Al and Ba–Pt sites was achieved over the Pt/BaO/Al_2O_3 surface when using Al_2O_3-nr as a support.This strong interaction among the multi-components of Pt/BaO/Al_2O_3-nr thus triggered the formation of surface nitrite and nitrate during the lean period, and also accelerated the reverse spillover of ad-NOxspecies onto the Pt surface, enhancing their reduction and leading to high NSR performance.展开更多
The applicability of a commercial Pt-Sn/Al2O3 isobutane dehydrogenation catalyst in dehydrogenation of propane was studied. Catalyst performance tests were carded out in a fixed-bed quartz reactor under different oper...The applicability of a commercial Pt-Sn/Al2O3 isobutane dehydrogenation catalyst in dehydrogenation of propane was studied. Catalyst performance tests were carded out in a fixed-bed quartz reactor under different operating conditions. Generally, as the factors improving propane conversion decrease the propylene selectivity, the optimal operating condition to maximize propylene yield is expected. The optimal condition was obtamed by the experimental design method. The investigated parameters were temperature, hydrogen/hydrocarbon （HE/HC） ratio and space velocity, being changed in three levels. Constrains such as the susceptibility of the catalyst components to sintering or phase transformation were also taken into account. Activity, selectivity and stability of the catalyst were considered as the measured response factors, while the space-time-yield （STY） was considered as the variable to be optimized due to its commercial interest. A STY of 16 mol.kg^-1.h^-1 was achieved under the optimal conditions of T= 620 ℃, H2/HC = 0.6 and, weight hourly space velocity （WHSV） = 2.2 h^-1. Single carbon-carbon bond rupture was found to be the main route for the formation of lower hydrocarbon byproducts.展开更多
基金supported by the Key Innovation Team of Science&Technology in Zhejiang Province,China(2011R50017)National HighTechnology Research and Development Program of China(863)(2013AA065005)~~
文摘分别通过自组装法(AS)和浸渍法(WI)制备得到纳米催化剂Pt/γ-Al2O3-AS和Pt/γ-Al2O3-WI,并用于评价甲苯、异丙醇、丙酮、乙酸乙酯等易挥发性有机物(VOCs)的氧化性能.通过各种表征手段探究了催化剂形态、结构及表面性质与催化剂氧化活性的关系.结果表明,Pt/γ-Al2O3-AS在低温下即可实现VOCs的完全氧化.在气体浓度(体积分数)为1000×10-6,空速为18000 m L·g-1·h-1的条件下,甲苯、异丙醇、丙酮、乙酸乙酯被Pt/γ-Al2O3-AS催化剂完全氧化的温度分别为130、135、145、215°C,展现出了优异的氧化性能,且具有很好的稳定性.该催化剂较高的比表面积、较小的Pt纳米粒径、较好的Pt纳米颗粒分散度、更好的低温还原效果及丰富的表面羟基是具有较高催化活性的重要因素.
基金supported by the National Natural Science Foundation of China (Nos.21673277 and 21637005)the National Key R&D Program of China (No.2017YFC0211105)+1 种基金the Science and Technology Program of Tianjin,China (No.16YFXTSF00290)the K.C.Wong Education Foundation
文摘Pt/BaO/Al_2O_3 catalysts with different BaO loadings prepared from Al_2O_3 nanorods(Pt/BaO/Al_2O_3-nr) and irregular Al_2O_3 nanoparticles(Pt/BaO/Al_2O_3-np) were investigated for NOx storage and reduction(NSR). The Pt/BaO/Al_2O_3 materials derived from Al_2O_3 nanorods always exhibited much higher NOx storage capacity(NSC) over the whole temperature range of 100–400°C than the corresponding Pt/BaO/Al_2O_3-np samples containing the same BaO loading, giving the maximum NSC value of 966.9 μmol/gcatat 400°C, 1.4 times higher than that of Pt/BaO/Al_2O_3-np. Higher catalytic performance of nanorod-supported NSR samples was also observed during lean-rich cyclic conditions(90 sec vs. 5 sec), giving more than 98% NOx conversion at 300–450°C over the Pt/BaO/Al_2O_3-nr sample with 15% BaO loading. To reveal this dependence on the shape of the support during the NSR process, a series of characterization techniques including the Brunauer–Emmett–Teller(BET) method,X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), H_2 temperature programmed reduction(H2-TPR), and in situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS) were also conducted. It was found that intimate contact of Ba–Al and Ba–Pt sites was achieved over the Pt/BaO/Al_2O_3 surface when using Al_2O_3-nr as a support.This strong interaction among the multi-components of Pt/BaO/Al_2O_3-nr thus triggered the formation of surface nitrite and nitrate during the lean period, and also accelerated the reverse spillover of ad-NOxspecies onto the Pt surface, enhancing their reduction and leading to high NSR performance.
基金Supported by the Petrochemical Research&Technology Co. of National Petrochemical Co.
文摘The applicability of a commercial Pt-Sn/Al2O3 isobutane dehydrogenation catalyst in dehydrogenation of propane was studied. Catalyst performance tests were carded out in a fixed-bed quartz reactor under different operating conditions. Generally, as the factors improving propane conversion decrease the propylene selectivity, the optimal operating condition to maximize propylene yield is expected. The optimal condition was obtamed by the experimental design method. The investigated parameters were temperature, hydrogen/hydrocarbon （HE/HC） ratio and space velocity, being changed in three levels. Constrains such as the susceptibility of the catalyst components to sintering or phase transformation were also taken into account. Activity, selectivity and stability of the catalyst were considered as the measured response factors, while the space-time-yield （STY） was considered as the variable to be optimized due to its commercial interest. A STY of 16 mol.kg^-1.h^-1 was achieved under the optimal conditions of T= 620 ℃, H2/HC = 0.6 and, weight hourly space velocity （WHSV） = 2.2 h^-1. Single carbon-carbon bond rupture was found to be the main route for the formation of lower hydrocarbon byproducts.
