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21.
研究了低温条件下单独臭氧及MgO催化臭氧化降解水中氨氮的效率和特征,并对其反应机制分别进行了探讨.结果表明,pH是影响臭氧和催化臭氧化除氨的重要因素,不仅影响溶液中NH_3与NH~+_4的比例和臭氧氧化氨氮的速率,还影响氧化产物种类,从而影响脱氮效果.10℃时,单独臭氧对水中氨氮的氧化降解效率随pH的升高而增大,pH≤9时整体降解效率不高,pH=9时仅为16.39%,而pH=10时达到41.77%.臭氧和·OH共同参与降解氨氮的过程.单独臭氧氧化氨氮生成氮气的选择性具有pH依赖性,并与Cl~-密切相关.pH低(≤9)时,氨氮多以NH~+_4形态存在,O_3与Cl~-反应生成ClO~-_x(x=1、3),再氧化NH~+_4,从而生成气态产物N_2或N_2O.MgO在低温条件下具有很强的催化臭氧化降解氨氮的能力且温度升高有利于反应的进行,0、10、20℃时,MgO催化臭氧化氨氮的效率分别为77.53%、80.17%、91.26%.此过程中,·OH参与反应的程度低,一部分氨氮降解依靠ClO~-_x氧化NH~+_4,而氨氮降解的主要途径为O_3对NH_3的直接氧化. 相似文献
22.
乙醇汽油车尾气中除了传统汽油车的三大常规污染物(CO、NO
23.
《环境科学学报(英文版)》2023,35(3):388-400
Removing large concentrations of organic pollutants from water efficiently and quickly under visible light is essential to developing photocatalytic technology and improving solar energy efficiency. This study used a simple hydrothermal method to prepare a non-metallic, S-doped NaTaO3 (S-NTO) photocatalyst, which was then loaded onto biochar (BC) to form a S-NTO/BC composite photocatalyst. After uniform loading onto BC, the S-NTO particles transformed from cubic to spherical. The photogenerated electron-hole pair recombination probability of the composite photocatalyst was significantly lower than those of the NTO particles. The light absorption range of the catalyst was effectively widened from 310 nm UV region to visible region. In addition, a dual-effect catalytic system was constructed by introducing peroxymonosulfate (PMS) into the environment of the pollution to be degraded. The Rhodamine B, Methyl Orange, Acid Orange 7, tetracycline, and ciprofloxacin degradation efficiency at 40 mg/L reached 99.6%, 99.2%, 84.5%, 67.1%, and 70.7%, respectively, after irradiation by a 40 W lamps for 90 min. The high-efficiency visible-light catalytic activity of the dual-effect catalytic system was attributed to doping with non-metallic sulfur and loading of catalysts onto BC. The development of this dual-effect catalytic system provides new ideas for quickly and efficiently solving the problem of high-concentration organic pollution in aqueous environments, rationally and fully utilizing solar energy, and expanding the application of photocatalytic technology to practice. 相似文献
24.
《环境科学学报(英文版)》2023,35(4):396-407
Based on the experimental and theoretical methods, the NO selective catalytic oxidation process was proposed. The experimental results indicated that lattice oxygen was the active site for NO oxide over the -MnO2(110) surface. In the theoretical study, DFT (density functional theory) and periodic slab modeling were performed on an -MnO2(110) surface, and two possible NO oxidation mechanisms over the surface were proposed. The non-defect -MnO2(110) surface showed the highest stability, and the surface Os (the second layer oxygen atoms) position was the most active and stable site. O2 molecule enhanced the joint adsorption process of two NO molecules. The reaction process, including O2 dissociation and O=N-O-O-N=O formation, was calculated to carry out the NO catalytic oxidation mechanism over -MnO2(110). The results showed that NO oxidation over the -MnO2(110) surface exhibited the greatest possibility following the route of O=N-O-O-N=O formation. Meanwhile, the formation of O=N-O-O-N=O was the rate-determining step. 相似文献
25.
《环境科学学报(英文版)》2023,35(4):459-469
A novel La-Co-O-C (LC-C) composites were prepared via a facile co-hydrothermal route with oxides and glycerol and further optimized for methane catalytic activity and thermal stability via component regulation. It was demonstrated that Co3O4 phase was the main component in regulation. The combined results of X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption of oxygen (O2-TPD), temperature-programmed reduction of hydrogen (H2-TPR), temperature-programmed desorption of ammonia/carbon dioxide (NH3/CO2-TPD) revealed that component regulation led to more oxygen vacancies and exposure of surface Co2+, lower surface basicity and optimized acidity, which were beneficial for adsorption of active oxygen species and activation of methane molecules, resulting in the excellent catalytic oxidation performance. Especially, the (3.5)LC-C (3.5 is Co-to-La molar ratio) showed the optimum activity and the T50 and T90 (the temperature at which the CH4 conversion rate was 50% and 90%, respectively) were 318 and 367°C, respectively. Using theoretical calculations and in situ diffuse reflection infrared Fourier transform spectroscopy characterization, it was also found that the catalytic mechanism changes from the “Rideal-Eley” mechanism to the “Two-term” mechanism depending on the temperature windows in which the reaction takes place. Besides, the use of the “Flynn-Wall-Ozawa” model in thermoanalytical kinetics revealed that component regulation simultaneously optimized the decomposition activation energy, further expanding the application scope of carbon-containing composites. 相似文献
26.
《环境科学学报(英文版)》2023,35(2):491-504
Ce1-xZrxO2 composite oxides (molar, x = 0-1.0, interval of 0.2) were prepared by a cetyltrimethylammonium bromide-assisted precipitation method. The enhancement of silver-species modification and catalytic mechanism of adsorption-transformation-desorption process were investigated over the Ag-impregnated catalysts for low-temperature selective catalytic oxidation of ammonia (NH3-SCO). The optimal 5 wt.% Ag/Ce0.6Zr0.4O2 catalyst presented good NH3-SCO performance with >90% NH3 conversion at temperature (T) ≥ 250°C and 89% N2 selectivity. Despite the irregular block shape and underdeveloped specific surface area (∼60 m2/g), the naked and Ag-modified Ce0.6Zr0.4O2 solid solution still obtained highly dispersed distribution of surface elements analyzed by scanning electron microscope-energy dispersive spectrometer (SEM-EDS) (mapping), N2 adsorption-desorption test and X-ray diffraction (XRD). H2 temperature programmed reduction (H2-TPR) and X-ray photoelectron spectroscopy (XPS) results indicated that Ag-modification enhanced the mobility and activation of oxygen-species leading to a promotion on CeO2 reducibility and synergistic Ag0/Ag+ and Ce4+/Ce3+ redox cycles. Besides, Ag+/Ag2O clusters could facilitate the formation of surface oxygen vacancies that was beneficial to the adsorption and activation of ammonia. NH3-temperature programmed desorption (NH3-TPD) showed more adsorption-desorption capacity to ammonia were provided by physical, weak- and medium-strong acid sites. Diffused reflectance infrared Fourier transform spectroscopy (DRIFTS) experiments revealed the activation of ammonia might be the control step of NH3-SCO procedure, during which NH3 dehydrogenation derived from NHx-species and also internal selective catalytic reduction (i-SCR) reactions were proposed. 相似文献
27.
28.
化学链燃烧中钙基载氧体CaSO4再生的氧化反应机理 总被引:1,自引:0,他引:1
在热重和红外联用进行等温实验的基础上,探讨了氧体积分数为10%、20%,970~1150℃温度范围内化学链燃烧过程中钙基载氧体再生(CaS)的氧化特性.结果显示,CaS氧化的直接产物主要为CaSO4,只有在诱导期生成极少量CaO和SO2;但CaSO4与CaS还可进一步反应,生成更多CaO和SO2.通过对氧气浓度和温度的实验条件改变,研究了CaSO4的转化率、转化速率,并辅以SO2析出速率分析,获得了CaSO4相对于CaO的瞬时选择性、CaSO4的收率和反应选择率.结果表明,钙基载氧体CaSO4再生过程氧化反应的适宜条件为温度970~1000℃以及较高的氧气气氛,这不仅可以抑制SO2的排放量从而得到较高的反应选择率,同时反应过程也具有较高的转化速率. 相似文献
29.
30.
铁基催化剂的微波水热处理对其SCR脱硝性能的影响 总被引:1,自引:0,他引:1
利用微波对共沉淀制备的铁铈钛复合氧化物催化剂前驱体进行水热处理,探讨了微波水热处理对铁基催化剂低温SCR脱硝性能的优化;并对微波水热处理条件的影响进行了正交分析.结果表明:对铁基催化剂前驱体进行微波水热处理,可提高其低温SCR脱硝性能,使其脱硝温度窗口向低温偏移;且微波水热处理的低温优化效果与催化剂中Fe/Ti摩尔比密切相关,Fe/Ti摩尔比越小,微波水热处理的低温优化越强;微波加热方式和微波辐射时间会影响微波水热处理对铁基催化剂SCR脱硝性能的低温优化;在相同微波辐射时间条件下,当P30逐渐变为P80,微波水热处理对铁基催化剂低温SCR脱硝的促进作用降低;在P30条件下,微波辐射15min使铁基催化剂具有最佳低温SCR脱硝活性. 相似文献