氧化物催化剂对非热等离子体催化降解甲苯的影响

考察了在干燥气氛下不同氧化物催化剂对非热等离子体催化降解甲苯的影响。从甲苯降解率、碳平衡、CO2选择性和O3去除4个方面,对比了氧化物催化剂的介电性能、表面供氧能力和比表面积与多孔结构对反应产生影响的强弱。结果表明,催化剂的介电性能有利于甲苯降解率、碳平衡和O3产量的提高,但对CO2选择性和O3去除的影响极小;一定能量密度下,催化剂比表面积与多孔结构对CO2选择性和O3去除所产生的影响要强于介电性能;催化剂表面供氧能力可明显促进反应的进行,其对反应所产生的影响要强于比表面积与多孔结构。     

Fe3O4/Ag磁性纳米颗粒去除水中的铅离子

采用水相共沉淀法制备小尺寸磁性Fe₃O₄纳米颗粒,以没食子酸作为还原剂和表面修饰剂,还原Ag[(NH₃)₂]⁺制备出Fe₃O₄/Ag磁性纳米颗粒。研究该磁性纳米颗粒对水溶液中铅离子的吸附行为,研究结果表明,pH为7.0,吸附温度30℃时可得到最好的处理效果,铅的去除率可达99.7%以上,Fe₃O₄/Ag颗粒吸附行为符合二级动力学模型(R² > 0.99)。该磁性纳米颗粒经过多次再生处理后,仍具有很好的吸附效果,表明Fe₃O₄/Ag在水处理方面拥有良好的应用前景。     

水泥窑协同处置过程中Pb、Cd的挥发特性

对铅、镉2种重金属的氧化物开展了热重实验、熟料煅烧以及熟料消解实验,以重金属的挥发率为主要指标,研究了水泥窑协同处置过程中铅、镉在等温条件下随时间的挥发特性。结果表明,2种重金属的挥发率均是随温度的升高,时间的增加而增大。Pb的挥发率为96%,Cd的挥发率达到98%,根据等温动力学及阿累尼乌斯方程,对Pb,Cd的挥发率随时间变化的规律进行动力学模拟,得到较好的线性拟合效果,其中,Pb挥发反应的表观活化能E为88.73 kJ/mol,Cd挥发反应可以分2个部分：1 200℃以下的表观活化能E为61 kJ/mol;1 250℃以上的表观活化能E为184.6 kJ/mol。     

响应面优化CCl4增强超声降解左旋氧氟沙星模拟废水

利用响应面优化实验设计方法对CCl₄增强超声降解左旋氧氟沙星模拟废水的影响因素进行探讨和分析,考察了溶液初始pH值、超声功率、左旋氧氟沙星初始浓度的影响。应用Box-Behnken中心组合设计得到一个二次多项式数学模型,确定了US/CCl₄降解左旋氧氟沙星的优化条件:初始pH值6.8,超声功率189 W,左旋氧氟沙星初始浓度为5 mg/L时,左旋氧氟沙星的去除率达到最大(82.99%)。经实验验证, 实际值与模型预测值吻合性良好,偏差仅为0.036%。     

堇青石负载Pd和过渡金属氧化物催化剂的表征及其对CO的催化氧化活性

以堇青石蜂窝陶瓷(CC)为载体,采用浸渍法制备了堇青石负载Pd和过渡金属混合氧化物催化剂,记作Pd-M-Mn(M=Cu,Co,Fe,Ni)/CC。实验结果表明:Pd-Co-Mn/CC催化剂的催化活性最高;随着Pd负载量的增加,CO转化率提高;当Pd负载量为1.00%时,反应温度为150℃时CO转化率达到98%,200℃时CO转化率达到100%;在反应温度150℃条件下,Pd-Co-Mn/CC催化剂(Pd负载量1.00%)的CO转化率在前30h内小幅度下降,随后稳定在90%以上,反应100h后,催化剂表面颜色由黑色变为棕褐色。     

利用钢铁盐酸酸洗废液在填料塔中制备FeCl3

以钢铁盐酸酸洗废液为原料,亚硝酸钠为催化剂,氧气为氧化剂,在填料塔中催化氧化制备三氯化铁。考察了反应温度、催化剂加入量和添加方式、循环流量等对制备三氯化铁的影响。实验结果表明,在优化的工艺条件为料液预热温度为60 ℃、催化剂加入量为钢铁盐酸酸洗废液总质量的0.30%、料液循环流量6.0 m³/h的条件下,反应80~120 min,酸洗废液中的Fe²⁺完全氧化为Fe³⁺。     

Projecting Climate Change Effects on Forest Net Primary Productivity in Subtropical Louisiana,USA

This study projected responses of forest net primary productivity (NPP) to three climate change scenarios at a resolution of 5 km × 5 km across the state of Louisiana, USA. In addition, we assessed uncertainties associated with the NPP projection at the grid and state levels. Climate data of the scenarios were derived from Community Climate System Model outputs. Changes in annual NPP between 2000 and 2050 were projected with the forest ecosystem model PnET-II. Results showed that forest productivity would increase under climate change scenarios A1B and A2, but with scenario B1, it would peak during 2011–2020 and then decline. The projected average NPP under B1 over the years from 2000 to 2050 was significantly different from those under A1B and A2. Forest NPP appeared to be primarily a function of temperature, not precipitation. Uncertainties of the NPP projection were due to large spatial resolution of the climate variables. Overall, this study suggested that in order to project effects of climate change on forest ecosystem at regional level, modeling uncertainties could be reduced by increasing the spatial resolution of the climate projections.     

Temperature-dependent sorption of polycyclic aromatic hydrocarbons on natural and treated sediments

In aqueous environment temperature is considered to play a significant role in the sorption process of polycyclic aromatic hydrocarbons (PAHs) and its influence on the sorption equilibrium is indicative of sorption energies and mechanisms. In this study, sorptions of five PAHs on three heterogeneous sorbents including one river sediment (YHR), one estuary sediment (YRD) and one treated sediment with organic matter removed (IM) were carried out at a range of temperature from 5 °C to 35 °C. Stronger sorptions were observed at lower temperatures, with the equilibrium sorption coefficient K_d increasing 2-5 times as the temperature decreases 30 °C. The increase of K_d value was attributed primarily to the change of PAH water solubility, which predicted 40-75% of the increase of K_d in the sorption process. To provide insight into the sorption mechanism, enthalpy change (ΔH_S) for the sorption process was calculated and the values were observed to be negative for all of the interactions, suggesting that the exothermal sorption of PAHs inversely dependents on temperature. Based on the values of ΔH_S, van der Waals forces were inferred as the main sorption mechanism for the PAHs, especially on the YHR sediment which contained more organic matter. For sorption of larger size PAHs on the sorbents with low organic matter, specific interactions were deduced to contribute to the overall sorption.     

Removal of Rhodamine B under visible irradiation in the presence of Fe⁰, H₂O₂, citrate and aeration at circumneutral pH

A new Vis-Fe⁰-H₂O₂-citrate-O₂ system comprising zero-valent iron, hydrogen peroxide, citrate anion and aeration at circumneutral pH under visible irradiation was studied. 21 μmol L⁻¹ of Rhodamine B (RhB) was chosen as the substrate to be tested. Experiments were conducted under conditions of 2.9 mmol L⁻¹ of H₂O₂, 12.6 g of Fe⁰ and 1.0 mmol L⁻¹ of citrate at pH 7.5. Results showed that, in 1 h reaction, 54% of RhB was removed with corresponding 26% of COD reduced. Meanwhile, the amount of released dissolved irons from Fe⁰ surface was found to be at a very low level as <5.4 μmol L⁻¹. Extinguishing tests with isopropanol suggested that RhB oxidation by hydroxyl radicals was the main process taken place in Vis-Fe⁰-H₂O₂-citrate-O₂ system, which accounted for 75% of substrate removal in 3 h reaction. Control and factor influencing experiments showed that the prohibitive extents of individual factor importance on RhB removal followed a decreasing order of Fe⁰ > H₂O₂ > citrate > Vis > O₂. This study showed an excellent system that could remove refractory organic compounds from water in laboratory researches, and also provided a good idea to reduce secondary contamination by dissolved irons in future investigations.     

Photodegradation of azithromycin in various aqueous systems under simulated and natural solar radiation: kinetics and identification of photoproducts

This article describes the photolysis of azithromycin, a macrolide antibiotic with reported occurrence in environmental waters, under simulated solar radiation. The photodegradation followed first-order reaction kinetics in five matrices examined. In HPLC water, the degradation rate was the slowest (half-life: 20 h), whereas in artificial freshwater supplemented with nitrate (5 mg L⁻¹) or humic acids (0.5 mg L⁻¹) the degradation of azithromycin was enhanced by factors of 5 and 16, respectively, which indicated the role of indirect photolysis involving the formation of highly reactive species. Following chromatographic separation on a UPLC system, the characterization of the transformation products was accomplished using high-resolution QqToF-MS analysis. The presence of seven photoproducts was observed and their formation was postulated to originate from (bis)-N-demethylation in the desosamine sugar, O-demethylation in the cladinose sugar, combinations thereof, as well as from hydrolytic cleavages of the desosamine and/or cladinose residue. Two of these photoproducts could also be detected in natural photodegradation process in river water which was spiked with azithromycin.