Ca_5(AsO_4)_3OH的溶解度与稳定性研究

通过在不同pH值,温度等条件下Ca5(AsO4)3OH的溶解,确定其稳定存在的pH值范围,得出它的溶度积和生成的自由能(ΔG0f)。结果表明,Ca5(AsO4)3OH在水中的溶解度和稳定范围与pH和温度有关,在酸性条件下(初始pH=2)它的溶解度较大,而且在水中的溶解度随着温度的升高而降低。利用PHREEQC程序计算确定Ca5(AsO4)3OH的溶度积为10-40.86,生成自由能ΔG0f为-5 063.53 kJ/mol。利用JADE5软件计算得到其晶格参数a=b=9.696,c=6.967和晶胞体积为567.304 3。     

用于CO2捕集的Mg(OH)2粉末溶解速率

氢氧化镁是一种正在研究的用于脱除烟气中低浓度CO2的化学吸收剂。为了掌握工业用氢氧化镁粉末的溶解速率,利用缓冲溶液,在不改变溶液体积的情况下对不同悬浊液浓度、溶液温度、溶液pH值和搅拌速率情况下的氢氧化镁粉末溶解速率进行了研究。提高悬浊液浓度、提高溶液温度、降低溶液pH值和提高搅拌速率均能增大氢氧化镁的溶解速率。悬浊液浓度从0.1 mol/L增加到1 mol/L时,溶解速率增大了2.2倍;温度从23℃增加到52℃时,溶解速率增大了4.3～9.5倍;pH值从9.8降低到6.6时,溶解速率增大了78～225倍;搅拌速率从350 r/min增加到700 r/min时,溶解速率增大了1～2倍。     

EDTA-（NH4）2FeSO4络合剂脱除烟气中的氮氧化物

络合脱硝法是近年来新型的脱除氮氧化物的方法之一,其中EDTA金属络合剂受到了广泛关注,而亚铁络合剂又具有很好的脱除氮氧化物的效果。考查了硫酸亚铁铵与EDTA形成的Fe（II）EDTA这种比较常见的EDTA金属络合剂对NO的吸收容量,并考查温度、络合剂浓度等对Fe（II）EDTA吸收NO的影响。研究结果表明：在相同的实验环境和实验条件下,对于影响Fe（II）EDTA吸收NO的因素最重要的是温度,其余依次为络合剂浓度、气体流速、氧含量、吸收液pH,最适宜吸收条件是反应温度50℃、络合剂浓度0．1mol／L、进气流速600mL／min、氧含量2％、吸收液pH=6。     

Secular trends of atmospheric methane (CH4)

Due partly to human activities the present yearly emissions of CH₄ exceed the atmospheric sinks, thus leading to a 1.2–1.9% per year atmospheric increase in the concentration of CH₄. New evidence based on studies of polar ice cores suggests that several hundred years ago the concentrations of CH₄ were perhaps only half of current values. These diverse findings are tied together in a single unified logistic model of atmospheric concentrations past, present and future. Using realistic growth rates of the sources of CH₄ caused by human activities, the model explains the concentrations and current growth rates. It also predicts that a doubling of CH₄ relative to present levels is possible given the long (9-year) atmospheric lifetime. Such increases of CH₄ concentrations may have already perturbed our global environment and may continue to do so in the future. The environmental effects include increased surface temperature of the earth, additional O₃ and CO in the clean non-urban atmosphere, depletions of tropospheric OH radicals, but perhaps also protection of the stratospheric ozone layer from destruction by man-made fluorocarbons.     

Comparative study of the oxidation of atrazine and acetone by H2O2/UV, Fe(III)/UV, Fe(iii)/H2O2/UV and Fe(II) or Fe(III)/H2O2

In this study, the rates of degradation of organic compounds by several AOPs (H₂O₂/UV, Fe(III)/UV, Fe(III)/H₂O₂/UV, Fe(II)/H₂O₂ and Fe(III)/H₂O₂) have been compared. Experiments were carried out at pH ≈ 3 (perchloric acid / sodium perchlorate solutions) and with UV reactors equipped with a low-pressure mercury vapour lamp (emission at 253.7 run). The data obtained with atrazine ([Atrazine]_o = 100 μg/L) showed that the rate of degradation of atrazine in very dilute aqueous solution is much more rapid with Fe(III)/UV than with H₂O₂/UV. Photo-Fenton process (Fe(III)/H₂O₂/UV) was found to be more efficient than H₂O₂/UV and Fe(II)/H₂O₂ for the mineralization of acetone ([Acetone]_o = 1 mM).     

V2O5-TiO2-AlF3/Al2O3催化臭氧化2,4-滴丙酸的氧化效能

为了提高有机物的臭氧化降解效率,工作中利用浸渍法制备了一种新型的三组分催化剂(记为V2O5-TiO2-AlF3/Al2O3)。催化臭氧化降解2,4-滴丙酸的实验结果表明,该催化剂能有效提高臭氧化的效率,体系可能遵循羟基自由基的作用机理。利用相对法计算结果表明,与单独臭氧化相比,V2O5-TiO2-AlF3/Al2O3催化臭氧化体系具有更大的Rct值。重复实验结果表明,该催化剂具有相对较好的稳定性。以上研究结果对推广催化臭氧化技术在实际废水处理中的应用具有重要的实际意义。     

Selective accumulation of chlorinated paraffins (C12 and C16) in the olfactory organ of rainbow trout

Three ¹⁴C-labelled polychloroalkanes (C₁₂ and C₁₆), representing low (23% Cl by weight), medium (51%), and highly (68%) chlorinated paraffin (CP) mixtures, were presented to rainbow trout via the water. The uptake in fat-rich tissues was positively correlated to the degree of chlorination of the preparations. Notably, all preparations gave rise to a high and selective uptake of radioactivity in the olfactory organ and gills. This selective radiolabelling may reflect a general ability of these organs to enrich xenobiotics from the surrounding water. The olfactory organ may be a hitherto unforseen target for toxic environmental pollutants in fish.     

Chemical degradation of chlorophenols with Fenton's reagent (Fe + H2O2)

Aqueous solutions of Fenton's reagent (Fe²⁺ + H₂O₂) have been used to effect the total decomposition of the chlorophenols: 2-chlorophenol, 3-chlorophenol, 4-chlorophenol, 3,4-dichlorophenol and 2,4,5-trichlorophenol. The mineralization of these chlorinated aromatic substrates to CO₂ and free Cl⁻ has been studied as a function of [Fe²⁺] and [HClO₄]. Increasing the concentration of Fe²⁺ enhances the decomposition process, while an increase in the concentration of HClO₄, inhibits the reaction. The presence of Fe³⁺ alone (without any Fe²⁺) with H₂O₂ has no effect on the degradation of the chlorophenols. In all cases, the stoichiometric quantity of free Cl⁻ was obtained at the completion of the decomposition reaction; but the rates of disappaearance of the chlorophenol and of the formation of the Cl⁻ are not similar. This suggests that some chlorinated aliphatic species may be formed as possible intemediates.     

The influence of engineered Fe2O3 nanoparticles and soluble (FeCl3) iron on the developmental toxicity caused by CO2-induced seawater acidification

An embryo development assay using a common test organism, the edible mussel (Mytilus galloprovincialis), exposed to both Fe₂O₃ nanoparticles and soluble FeCl₃ at 3 acidic pHs, has provided evidence for the following: (1) CO₂ enriched seawater adjusted to pH projections for carbon capture leakage scenarios (CCS) significantly impaired embryo development; (2) under natural pH conditions, no significant effect was detected following exposure of embryos to Fe, no matter if in nano- or soluble form; (3) at pH of natural seawater nano-Fe particles aggregate into large, polydisperse and porous particles, with no biological impact detected; (4) at pH 6 and 7, such aggregates may moderate the damage associated with CO₂ enrichment as indicated by an increased prevalence of normal D-shell larvae when nano-Fe was present in the seawater at pH 7, while soluble iron benefited embryo development at pH 6, and (5) the observed effects of iron on pH-induced development toxicity were concentration dependent.     

微波促进含Cr(VI)-H2O2体系降解甲基橙溶液的研究

研究了微波辐射下Cr(VI)－H₂O₂催化降解甲基橙溶液的行为，探索了微波功率、微波辐射时间、pH值、H₂O₂浓度、Cr(VI)等对甲基橙溶液脱色率和COD去除率的影响。研究结果表明，Cr(VI)-H₂O₂能形成类Fenton体系；微波辐射可提高H₂O₂产生羟基自由基(·OH)的效率。1000 mg/L的甲基橙溶液，在Cr(VI)浓度为10.0 mmol/L、pH值为2.5、H₂O₂浓度为20.0 mmol/L、微波功率为700W下加热2 min，甲基橙溶液的脱色率为99.2%，COD去除率为82.8%。     

UV/H2O2/Fe-FeOxH2x-3和UV/H2O2工艺降解水中富里酸的研究

采用硼氢化钠还原法制备核-壳结构的Fe-FeO_xH_2x-3复合材料，研究了富里酸在UV/H₂O₂和UV/H₂O₂/Fe-FeO_xH_2x-3两种不同反应体系下的降解情况。结果表明，核-壳结构Fe-FeO_xH_2x-3的存在，提高了UV/H₂O₂降解富里酸的反应速率，TOC去除达到84%。采用XAD树脂吸附法对反应前后的富里酸进行化学分级表征，结果表明，富里酸经反应后憎水酸（HoA）、弱憎水酸（WHoA）和憎水中性物质（HoN）都有所减少，进而转化为亲水性物质（HiM）；用超滤膜法对富里酸进行物理分级表征，考察了富里酸在反应前后分子量分布的变化情况。同时，富里酸经过反应后生成的中间产物降低了三氯甲烷生成趋势。     

Toxicity of TiO2, ZrO2, Fe,Fe2O3, and Mn2O3 nanoparticles to the yeast, Saccharomyces cerevisiae

The growing application of engineered nanomaterials is leading to an increased occurrence of nanoparticles (NPs) in the environment. Thus, there is a need to better understand their potential impact on the environment. This study evaluated the toxicity of nanosized TiO₂, ZrO₂, Fe⁰, Fe₂O₃, and Mn₂O₃ towards the yeast Saccharomyces cerevisiae based on O₂ consumption and cell membrane integrity. In addition, the state of dispersion of the nanoparticles in the bioassay medium was characterized.     

倒置A~2/O-MBR(平板膜)处理城市污水的中试研究

针对城市生活污水,研究了两点进水倒置A2/O-MBR(平板膜)系统(以下简称系统)对COD、NH+4-N、TN、TP、出水SS影响。结果表明,该系统对COD、NH+4-N具有较高的去除率,出水符合GB18918-2002中一级A标准;当混合液回流比为200%时,系统出水TN浓度小于15 mg/L;正常排泥后,系统对TP的去除率达83%左右;平板膜破损会导致出水SS、COD会受到影响。膜对COD、TP、SS有直接截留作用,由于系统出水几乎没有固体损失,可以精确控制污泥龄,有利于世代周期较长的硝化菌和反硝化菌生长;系统中的污泥浓度可以提高至15 000 mg/L,此时,即使进水量提高0.5倍,出水水质仍保持良好。     

H2O和SO2对V2O5-WO3/TiO2催化剂催化氧化NO的影响

研究了在120℃的反应温度下,H2O和SO2对V2O5-WO3TiO2催化剂选择性催化氧化(SCO)NO的影响.结果表明,在H2O和SO2存在的情况下催化剂失活很快,停止通入H2O和SO2后活性不能恢复,但在加热到250℃后催化活性基本恢复.FT-IR分析表明,催化剂表面形成了金属硝酸盐和Ti的硫酸盐,对催化活性有一定...     

Fe2O3-Cr2O3/TiO2系列催化剂的结构和脱硝性能

研究以纳米TiO2为载体,浸渍负载过渡金属氧化物,以CO为还原剂的脱硝催化剂的脱硝性能。实验中以计算量的Ni(NO3)2和Fe(NO3)3混合溶液浸渍纳米TiO2粉末,室温下搅拌30 min至混合均匀,放入旋转蒸发器中,70℃下至水分蒸干为止;所得粉末在550℃下、空气气氛中焙烧4 h即得所需催化剂。用以上方法分别制备2%Fe2O3-10%Cr2O3/TiO2、4%Fe2O3-8%Cr2O3/TiO2、6%Fe2O3-6%Cr2O3/TiO2、8%Fe2O3-4%Cr2O3/TiO2与10%Fe2O3-2%Cr2O3/TiO2等5种催化剂样品。实验结果表明,制备的催化剂具有较好的结构,分散较为均匀。对于CO+NO反应,Fe2O3-Cr2O3/TiO2系列催化剂具有较好的催化活性,NO的转化率都达到了100%。其中,10%Fe2O3-2%Cr2O3/TiO2样品具有最好的低温活性,H2-TPR结果表明,这是由于10%Fe2O3-2%Cr2O3/TiO2催化剂更易于被CO预还原。     

Gene expression responses of paper birch (Betula papyrifera) to elevated CO2 and O3 during leaf maturation and senescence

Gene expression responses of paper birch (Betula papyrifera) leaves to elevated concentrations of CO₂ and O₃ were studied with microarray analyses from three time points during the summer of 2004 at Aspen FACE. Microarray data were analyzed with clustering techniques, self-organizing maps, K-means clustering and Sammon's mappings, to detect similar gene expression patterns within sampling times and treatments. Most of the alterations in gene expression were caused by O₃, alone or in combination with CO₂. O₃ induced defensive reactions to oxidative stress and earlier leaf senescence, seen as decreased expression of photosynthesis- and carbon fixation-related genes, and increased expression of senescence-associated genes. The effects of elevated CO₂ reflected surplus of carbon that was directed to synthesis of secondary compounds. The combined CO₂ + O₃ treatment resulted in differential gene expression than with individual gas treatments or in changes similar to O₃ treatment, indicating that CO₂ cannot totally alleviate the harmful effects of O₃.     

O3/H2O2法去除浮选药剂丁基黄药

采用O3/H2O2法去除水中丁基黄药,考察了H2O2/O3摩尔比、pH值、丁基黄药初始浓度、温度和自由基抑制剂对丁基黄药的去除效果的影响。结果表明,在相同O3投加量下,H2O2量越大,丁基黄药去除率越高。pH值为7～9,温度在293～303 K的范围内,O3/H2O2对丁基黄药都有很高的去除率。碳酸氢根和叔丁醇能在一定程度上降低丁基黄药的降解效率。研究还发现,在O3和H2O2投加量相同的条件下,H2O2多次投加对水中丁基黄药的处理效果明显优于一次性投加。GC/MS分析表明,O3/H2O2氧化丁基黄药氧化产物为羧酸类物质。     

粗MnSO4溶液中MnS2O6的去除条件研究

用软锰矿吸收SO₂生成MnSO₄时会伴随有副产物MnS₂O₆生成。产品中MnS₂O₆的存在会降低硫酸锰产品质量,同时会缓慢释放出SO₂气体污染环境。本文用单因素实验方法研究了粗MnSO₄溶液中MnS₂O₆的最优去除条件。研究结果显示,软锰矿用量为12.2 g,硫酸加入量为20 mL、反应温度100℃、反应时间3 h、搅拌速度500 r/min,MnS₂O₆的去除率可达91%以上。其最终产品能达到GB1622-1986一级品标准。     

O3/H2O2降解阿特拉津影响因素研究

采用O3/H2O2氧化去除水中内分泌干扰物阿特拉津,考察了反应条件及水质对去除的影响,并对反应机制进行了初步探讨。阿特拉津初始浓度2 mg/L,投量为7.5 mg/L的O₃单独氧化去除率为27.2%;相同O₃投量下,控制H₂O₂/O₃摩尔比为0.75,5 min阿特拉津的去除率最高可达96.5%;pH 值为7.5～8.5,温度在25～40℃的范围内,都维持了较高的去除率,表明H₂O₂/O₃体系对阿特拉津的去除效果良好,降解速度快,反应条件温和。0.5 mg/L的腐殖酸,对阿特拉津的去除影响不大,腐殖酸浓度为1、2和5 mg/L时,平均去除率分别为63.4%、50.7%和30.2%;碳酸氢钠的浓度为50和200 mg/L时,去除率分别为88.1%和73.8%,说明水质对阿特拉津的去除影响较大。叔丁醇的浓度为5和20 mg/L时,阿特拉津的去除率分别降低到44.7%和27.5%,去除率随自由基抑制剂叔丁醇增加而降低,说明H₂O₂/O₃降解阿特拉津主要为该体系产生的羟基自由基的贡献。