本课题制备了一种F掺杂铜氧化物负载活性炭新型复合催化剂,并以此构建三维电极电Fenton体系。为探究此三维电极电Fenton体系对邻硝基苯酚(2-NP)降解的最佳条件,本实验对比了活性炭(GAC)、F掺杂铜氧化物负载活性炭复合催化剂(F/CuOx-GAC...本课题制备了一种F掺杂铜氧化物负载活性炭新型复合催化剂,并以此构建三维电极电Fenton体系。为探究此三维电极电Fenton体系对邻硝基苯酚(2-NP)降解的最佳条件,本实验对比了活性炭(GAC)、F掺杂铜氧化物负载活性炭复合催化剂(F/CuOx-GAC)、未掺杂F的铜氧化物负载活性炭复合催化剂(CuOx-GAC)对2-NP降解情况。并以降解效果最优的催化剂为基础,分别对反应时间、pH值、极板间距、电流密度、电极投加量、电解质浓度、曝气速率这些因素进行了单因素实验。结果表明,最佳实验条件为2 g催化剂、pH = 4、电极间距为3 cm、电流密度为20 mA/cm2、电解质浓度为30 mM、曝气速率为1.25 L/min,在该条件下反应3 h后体系2-NP去除率为98.12%。其中,在一定范围内电流密度与2-NP的去除率成正比,催化剂的量、电极间距在合适时,电流效率和传质效能达到平衡最高点。此外,还通过不同体系对比、催化剂表征、自由基猝灭,初步探明了所构建的三维电极电Fenton体系对2-NP的降解机制,并进一步验证其高效性。In this paper, a novel composite catalyst of F-doped copper oxide supported activated carbon was prepared, and a three-dimensional electrode electro-Fenton system was constructed. In order to explore the optimal conditions for the degradation of o-nitrophenol (2-NP) by this three dimensional electrode electro-Fenton system, this experiment compared the degradation of 2-NP by activated carbon (GAC), F-doped copper oxide supported activated carbon composite catalyst (F/CuOx-GAC), and undoped copper oxide supported activated carbon composite catalyst (CuOx-GAC). Based on the catalyst with the best degradation effect, the single-factor experiments were carried out on the factors of reaction time, pH value, plate spacing, current density, electrode dosage, electrolyte concentration, and aeration rate. The results showed that the optimal experimental conditions were 2 g catalyst, pH = 4, electrode spacing of 3 cm, current density of 20 mA/cm2, electrolyte concentration of 30 mM, and aeration rate of 1.25 L/min. Under these conditions, the removal rate of 2-NP in the system was 98.12% after 3 h of reaction. In a certain range, the current density is proportional to the removal rate of 2-NP, and the current efficiency and mass transfer efficiency reach the highest point of balance when the amount of catalyst and electrode spacing are appropriate. In addition, through the comparison of different systems, catalyst characterization, and radical quenching, the degradation mechanism of 2-NP by the constructed three-dimensional electrode electro-Fenton system was preliminarily proved, and its efficiency was further verified.展开更多
V2O5- SiO2（VSiO） supported Cu- Ni- K2O catalysts for the synthesis of dimethyl carbonate were prepared using isovolumic impregnation. Based on TPR,TPD, IR and micro- reactor techniques, the effect of K2O on the adso...V2O5- SiO2（VSiO） supported Cu- Ni- K2O catalysts for the synthesis of dimethyl carbonate were prepared using isovolumic impregnation. Based on TPR,TPD, IR and micro- reactor techniques, the effect of K2O on the adsorption and reaction of CO2 and CH3OH on the catalyst were characterized. The results show that addition of K2O exerts obvious influence on the charge distribution of the active sites on Cu- Ni/VSiO catalyst,increases the intensities of CO2 horizontal adsorption state, while that of the dissociation state of methanol descends. When the ratio of K is above 15％ , K2CO3 is formed on the catalyst. Moreover,the main reaction products of CO2 and CH3OH on Cu- Ni- K2O/VSiO catalyst are still DMC, H2O, CO and CH2O,and with the addition of K2O, the conversion of reactants rise, but the selectivity of by- products decreases.展开更多
文摘本课题制备了一种F掺杂铜氧化物负载活性炭新型复合催化剂,并以此构建三维电极电Fenton体系。为探究此三维电极电Fenton体系对邻硝基苯酚(2-NP)降解的最佳条件,本实验对比了活性炭(GAC)、F掺杂铜氧化物负载活性炭复合催化剂(F/CuOx-GAC)、未掺杂F的铜氧化物负载活性炭复合催化剂(CuOx-GAC)对2-NP降解情况。并以降解效果最优的催化剂为基础,分别对反应时间、pH值、极板间距、电流密度、电极投加量、电解质浓度、曝气速率这些因素进行了单因素实验。结果表明,最佳实验条件为2 g催化剂、pH = 4、电极间距为3 cm、电流密度为20 mA/cm2、电解质浓度为30 mM、曝气速率为1.25 L/min,在该条件下反应3 h后体系2-NP去除率为98.12%。其中,在一定范围内电流密度与2-NP的去除率成正比,催化剂的量、电极间距在合适时,电流效率和传质效能达到平衡最高点。此外,还通过不同体系对比、催化剂表征、自由基猝灭,初步探明了所构建的三维电极电Fenton体系对2-NP的降解机制,并进一步验证其高效性。In this paper, a novel composite catalyst of F-doped copper oxide supported activated carbon was prepared, and a three-dimensional electrode electro-Fenton system was constructed. In order to explore the optimal conditions for the degradation of o-nitrophenol (2-NP) by this three dimensional electrode electro-Fenton system, this experiment compared the degradation of 2-NP by activated carbon (GAC), F-doped copper oxide supported activated carbon composite catalyst (F/CuOx-GAC), and undoped copper oxide supported activated carbon composite catalyst (CuOx-GAC). Based on the catalyst with the best degradation effect, the single-factor experiments were carried out on the factors of reaction time, pH value, plate spacing, current density, electrode dosage, electrolyte concentration, and aeration rate. The results showed that the optimal experimental conditions were 2 g catalyst, pH = 4, electrode spacing of 3 cm, current density of 20 mA/cm2, electrolyte concentration of 30 mM, and aeration rate of 1.25 L/min. Under these conditions, the removal rate of 2-NP in the system was 98.12% after 3 h of reaction. In a certain range, the current density is proportional to the removal rate of 2-NP, and the current efficiency and mass transfer efficiency reach the highest point of balance when the amount of catalyst and electrode spacing are appropriate. In addition, through the comparison of different systems, catalyst characterization, and radical quenching, the degradation mechanism of 2-NP by the constructed three-dimensional electrode electro-Fenton system was preliminarily proved, and its efficiency was further verified.
文摘V2O5- SiO2（VSiO） supported Cu- Ni- K2O catalysts for the synthesis of dimethyl carbonate were prepared using isovolumic impregnation. Based on TPR,TPD, IR and micro- reactor techniques, the effect of K2O on the adsorption and reaction of CO2 and CH3OH on the catalyst were characterized. The results show that addition of K2O exerts obvious influence on the charge distribution of the active sites on Cu- Ni/VSiO catalyst,increases the intensities of CO2 horizontal adsorption state, while that of the dissociation state of methanol descends. When the ratio of K is above 15％ , K2CO3 is formed on the catalyst. Moreover,the main reaction products of CO2 and CH3OH on Cu- Ni- K2O/VSiO catalyst are still DMC, H2O, CO and CH2O,and with the addition of K2O, the conversion of reactants rise, but the selectivity of by- products decreases.
