金属掺杂纳米TiO2薄膜的制备和抗菌性能研究

采用sol—gel法在载玻片表面制备了Ce,Cu,i．a,Ag掺杂的锐铁矿相TiO2薄膜,并通过SEM,XRD．FT—IR及UVVIS进行了表征,比较了薄膜的抗菌性能．UV—VIS研究表明,金属掺杂纳米TiO2薄膜在近紫外区吸光度有明显提高。抗菌实验表明掺Ag的TiO2薄膜抗菌效果最佳。     

Selective removal of 2,4-dichlorophenoxyacetic acid from water by molecularly-imprinted amino-functionalized silica gel sorbent

A molecularly-imprinted amino-functionalized sorbent for selective removal of 2,4-dichlorophenoxyacetic acid(2,4-D) was prepared by a surface imprinting technique in combination with a sol-gel process.The 2,4-D-imprinted amino-functionalized silica sorbent was characterized by FT-IR,nitrogen adsorption and static adsorption experiments.The selectivity of the sorbent was investigated by a batch competitive binding experiment using an aqueous 2,4-D and 2,4-dichlorophenol(2,4-DCP) mixture or using an aqueous 2...     

Degradation and detoxification of microcystin-LR in drinking water by sequential use of UV and ozone

Microcystins (MCs) produced by cyanobacteria are strong hepatotoxins and classified as possible carcinogens.MCs pose a considerable threat to human health through tainted drinking and surface waters.Herein filtrated water from a waterworks in Harbin,China,was spiked with microcystin-LR (MC-LR) extracted from a toxic scum of microcystis aeruginosa,and the spiked sample waters were treated using UV irradiation with consequent ozonation process (UV/O3),compared with ozonation at a dose range commonly applied in water treatment plants,UV irradiation at 254 nm and UV irradiation combined with ozonation (UV+O3),respectively.The remaining of toxins were analyzed using high-performance liquid chromatography and also determined using a protein phosphatase type 2A inhibition assay,which was utilized to evaluate the reduction in toxicity.Results indicated that in comparison to other three processes (O3,UV,and UV+O3),UV/O 3 process could effectively decrease both the concentration and toxicity of MC-LR at 100 μg/L level after 5 min UV irradiation with consequent 5 min ozonation at 0.2 mg/L (below 1 μg/L),while 0.5 mg/L ozone dose was required for the level below 0.1 μg/L.The addition of an UV treatment step to the existing treatment train may induce significant transformation of micropollutants and breaks down the natural organic matters into moieties unfavorable for ozone decomposition,stabilizing the ozone residual.These findings suggested that sequential use of UV and ozone may be a suitable method for the removal of these potentially hazardous microcystins from drinking water.     

纳米催化剂Pd/SnO_2的制备及催化还原硝酸盐反应的调控

采用热分解法制备了SnO2载体,并用浸渍法制备了Pd/SnO2催化剂.同时,采用X射线衍射仪(XRD)、透射电镜(TEM)、扫描电镜(SEM)及BET比表面积仪等对所制载体和催化剂材料进行了分析表征.结果表明,热分解法和浸渍法都能够获得纳米材料,SnO2及Pd/SnO2的粒径均在9～10nm左右,比表面积分别达到144.99m·2g-1和147.36m·2g-1.在以甲酸为还原剂的Pd/SnO2催化还原硝酸盐体系中,在Pd与SnO2负载比为2%～7%,反应温度为20～50℃和甲酸投加量4.0～24.0mmol·L-1的条件下,催化活性为0.70～9.48mg·min-·1g-1,且催化活性随着负载比、温度和甲酸投加量的增大而增大,随着pH的升高先升后降,最佳pH为3.反应温度升高及pH降低都能够提高Pd/SnO2的选择性.甲酸-Pd/SnO2催化还原硝酸盐体系中还原反应的调控策略为:反应温度宜控制在40～50℃内,这样可同时获得较高的催化活性和选择性,温度过高对催化活性和选择性影响很小,温度过低则会同时降低催化活性和选择性;控制pH为3时,可以获得最大的催化活性及较好的选择性,pH升高会降低Pd/SnO2的催化活性和选择性,pH降低会导致催化活性迅速降低,但对选择性影响不大;甲酸与硝酸盐的物质的量比宜大于4:1,此时可以有效地抑制pH的上升,同时获得较高的催化活性和选择性,甲酸与硝酸盐的物质的量比小于4:1时,会同时降低Pd/SnO2的催化活性和选择性.     

A comparative investigation of NdSrCu_(1-x) Co_x O_(4-δ) and Sm_(1.8) Ce_(0.2) Cu_(1-x) Co_x O_(4-δ) (x:0–0.4) for NO decomposition

A series of single-phase T-structured NdSrCu 1-x Co x O 4-δ with oxygen vacancies and T -structured Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ (x: 0–0.4) with oxygen excess were prepared using ultrasound-assisted citric acid complexing method, and characterized by means of techniques such as thermogravimetric analysis and NO temperature-programmed desorption (NO-TPD). The catalytic activities of these materials were evaluated for the decomposition of NO. It was found that the NdSrCu 1-x Co x O 4-δ catalysts were of oxygen vacancies whereas the Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ ones possessed excessive oxygen (i.e., over-stoichiometric oxygen); with a rise in Co doping level, the oxygen vacancy density of NdSrCu 1-x Co x O 4-δ decreased while the over-stoichiometric oxygen amount of Sm 1.8 Ce 0.2 Cu 1-x Co x O 4-δ increased. The NO-TPD results revealed that NO could be activated much easier over the oxygen-deficient perovskite-like oxides than over the oxygen-excessive perovskite-like oxides, with the NdSrCuO 3.702 catalyst showing the best efficiency in activating NO molecules. Under the conditions of 1.0% NO/helium, 2800 hr -1 , and 600–900°C, the catalytic activity of NO decomposition followed the order of NdSrCuO 3.702 NdSrCu 0.8 Co 0.2 O 3.736 NdSrCu 0.6 Co 0.4 O 3.789 Sm 1.8 Ce 0.2 Cu 0.6 Co 0.4 O 4.187 Sm 1.8 Ce 0.2 Cu 0.8 Co 0.2 O 4.104 Sm 1.8 Ce 0.2 CuO 4.045 , in concord with the sequence of decreasing oxygen vacancy or oxygen excess density. Based on the results, we concluded that the higher oxygen vacancy density and the stronger Cu 3+ /Cu 2+ redox ability of NdSrCu 1-x Co x O 4-δ account for the easier activation of NO and consequently improve the catalytic activity of NO decomposition over the catalysts.     

Catalytic performance of Fe3O4-CoO/Al2O3 catalyst in ozonation of 2-(2,4-dichlorophenoxy)propionic acid, nitrobenzene and oxalic acid in water

Fe3O4-CoO/Al2O3 catalyst was prepared by incipient wetness impregnation using Fe(NO3) 3·9H2O and Co(NO3) 2·6H2O as the precursors,and its catalytic performance was investigated in ozonation of 2-(2,4-dichlorophenoxy) propionic acid(2,4-DP) ,nitrobenzene and oxalic acid.The experimental results indicated that Fe3O4-CoO/Al2O3 catalyst enabled an interesting improvement of ozonation eciency during the degradation of each organic pollutant,and the Fe3O4-CoO/Al2O3 catalytic ozonation system followed a radical-type mechanism.The kinetics of ozonation alone and Fe3O4-CoO/Al2O3 catalytic ozonation of three organic pollutants in aqueous solution were discussed under the mere consideration of direct ozone reaction and OH radical reaction to well investigate its performance.In the catalytic ozonation of 2,4-DP,the apparent reaction rate constants(k) were determined to be 1.456×10-2 min-1 for ozonation alone and 4.740×10-2 min-1 for O3/Fe3O4-CoO/Al2O3.And O3/Fe3O4-CoO/Al2O3 had a larger Rct(6.614×10-9) calculated by the relative method than O3 did(1.800×10-9) ,showing O3/Fe3O4-CoO/Al2O3 generated more hydroxyl radical.Similar results were also obtained in the catalytic ozonation of nitrobenzene and oxalic acid.The above results demonstrated that the catalytic performance of Fe3O4-CoO/Al2O3 in ozonation of studied organic substance was universal to a certain degree.     

Iron-doped Mn-Ce/TiO2 catalyst for low temperature selective catalytic reduction of NO with NH3

The catalysts of iron-doped Mn-Ce/TiO 2(Fe-Mn-Ce/TiO 2) prepared by sol-gel method were investigated for low temperature selective catalytic reduction(SCR) of NO with NH 3.It was found that the NO conversion over Fe-Mn-Ce/TiO 2 was obviously improved after iron doping compared with that over Mn-Ce/TiO 2.Fe-Mn-Ce/TiO 2 with the molar ratio of Fe/Ti = 0.1 exhibited the highest activity.The results showed that 96.8% NO conversion was obtained over Fe(0.1)-Mn-Ce/TiO 2 at 180°C at a space velocity of 50,000 hr 1.Fe-Mn-Ce/TiO 2 exhibited much higher resistance to H 2 O and SO 2 than that of Mn-Ce/TiO 2.The properties of the catalysts were characterized using X-ray diffraction(XRD),N 2 adsorption,temperature programmed desorption(NH 3-TPD and NOx-TPD),and Xray photoelectron spectroscopy(XPS) techniques.BET,NH3-TPD and NOx-TPD results showed that the specific surface area and NH3 and NOx adsorption capacity of the catalysts increased with iron doping.It was known from XPS analysis that iron valence state on the surface of the catalysts were in Fe3+ state.The doping of iron enhanced the dispersion and oxidation state of Mn and Ce on the surface of the catalysts.The oxygen concentrations on the surface of the catalysts were found to increase after iron doping.Fe-Mn-Ce/TiO2 represented a promising catalyst for low temperature SCR of NO with NH3 in the presence of H2 O and SO2.     

Cover crop effects on nitrous oxide emission from a manure-treated Mollisol

Agriculture contributes 40–60% of the total annual N₂O emissions to the atmosphere. Development of management practices to reduce these emissions would have a significant impact on greenhouse gas levels. Non-leguminous cover crops are efficient scavengers of residual soil NO₃, thereby reducing leaching losses. However, the effect of a grass cover crop on N₂O emissions from soil receiving liquid swine manure has not been evaluated. This study investigated: (i) the temporal patterns of N₂O emissions following addition of swine manure slurry in a laboratory setting under fluctuating soil moisture regimes; (ii) assessed the potential of a rye (Secale cereale L.) cover crop to decrease N₂O emissions under these conditions; and (iii) quantified field N₂O emissions in response to either spring applied urea ammonium nitrate (UAN) or different rates of fall-applied liquid swine manure, in the presence or absence of a rye/oat winter cover crop. Laboratory experiments investigating cover crop effects N₂O emissions were performed in a controlled environment chamber programmed for a 14 h light period, 18 °C day temperature, and 15 °C night temperature. Treatments with or without a living rye cover crop were treated with either: (i) no manure; (ii) a phosphorus-based manure application rate (low manure): or (iii) a nitrogen-based manure application rate (high manure). We observed a significant reduction in N₂O emissions in the presence of the rye cover crop. Field experiments were performed on a fine-loamy soil in Central Iowa from October 12, 2005 to October 2, 2006. We observed no significant effect of the cover crop on cumulative N₂O emissions in the field. The primary factor influencing N₂O emission was N application rate, regardless of form or timing. The response of N₂O emission to N additions was non-linear, with progressively more N₂O emitted with increasing N application. These results indicate that while cover crops have the potential to reduce N₂O emissions, N application rate may be the overriding factor.     

pH和铜离子对微囊藻毒素-LR荧光免疫检测的影响与消除

研究了pH和铜离子对倏逝波全光纤免疫传感器检测微囊藻毒素-LR（MC-LR）的影响及其消除措施.研究表明,过酸或过碱条件对MC-LR免疫检测均有较强烈的影响,当pH<6或pH>8时,系统检测的信号随pH的降低或增大明显下降;而当pH在6～8之间时,检测标准曲线的IC₅₀为1.01～1.04 μg/L,检测区间在0.12～10.5 μg/L之间,较适合MC-LR的检测.低浓度铜离子对MC-LR免疫检测的影响不大,当CuSO₄浓度>5 mg/Ｌ时,系统检测荧光信号明显下降,而当CuSO₄浓度达到10 mg/Ｌ时,系统检测信号下降70％以上.在预反应混合物中添加1%的螯合剂EDTA,能有效抑制铜离子对免疫检测的影响.     

温度对好氧颗粒污泥吸附铅离子的影响

由活性污泥培养得到好氧颗粒污泥,研究了温度对好氧颗粒污泥吸附Pb²⁺的影响.结果表明,好氧颗粒污泥主要含有C、H、N、O、P等元素,其经验结构式为C_5.7H_10.9O3.9NS_0.04.好氧颗粒污泥表面主要由球状细菌组成,具有明显的孔隙结构.在20～40℃时,Pb²⁺在好氧颗粒污泥上的吸附过程可以由Langmuir和Freundlich等温方程进行拟合（R²>0.914）.Pb2+最大吸附量Qmax由80.65 mg·g-1（20℃）增至97.09　mg·g-1（40℃）.吸附过程的表观自由能变ΔG<0、 ΔH>0、 ΔS>0,表明Pb2+在好氧颗粒污泥表面的吸附为吸热、熵增的自发过程.红外扫描分析(FTIR)结果表明,吸附过程Pb2+主要与—OH、蛋白质中的—COOH以及PO发生作用,与含氮官能团无关.