Purification and characterization of Al13 species in coagulant polyaluminum chloride

Nano-Al₁₃ was separated and purified by four methods to investigate its characteristic, and was analyzed by Al-Ferron timed complexation spectrophotometer,²⁷ Al-NMR (nuclear magnetic resonance), and transmission electron microscopy (TEM). Coagulation efficiency of nano-Al₁₃, polyaluminum chloride (PAC), and AlCl₃ in synthetic water were also investigated by jar test. The dynamic process and aggregation state of kaolin suspensions coagulating with nano-Al₁₃, PAC, and AlCl₃ were also investigated. The experimental results indicated that the efficiency of gel column chromatography method was the highest for separating PAC solution with low Al concentration. Ethanol and acetone method was simple and could separated PAC solution with different Al concentrations, while silicon alkylation white block column chromatography method could separate PAC solution only with low Al concentration. The SO₄²−/Ba²⁺ displacement method could separate PAC solution with high Al concentration, but extra inorganic cation and anion could be introduced into the solution during the separation. The coagulation efficiency and dynamic experimental results showed that nano- Al₁₃ with a high positive-charged species was the main species of electric neutralization in coagulation process, and it could reduce the turbidity and increase the effective particles collision rate efficiently in coagulation process. Its coagulation speed and the particle size of coagulant formed were of greatest value in this study.     

聚合氯化铝中纳米Al13电荷特性及其混凝效果

采用聚丙烯酰胺凝胶柱层析法分离纯化聚合氯化铝(PAC)中的Al₁₃形态,并采用Al-Ferron逐时络合比色法和ZATESIZER 3000HSA测定仪对分离所得纳米Al₁₃形态以及AlCl₃和PAC进行了分析表征和电荷特性的对比性研究;采用烧杯实验法对3个样品处理实际和模拟水样的混凝效果进行了对比性研究.Al-Ferron逐时络合比色法的结果表明,采用层析法分离可得到含量99%左右的纳米Al₁₃形态;电荷特性和混凝效果研究结果表明纳米Al₁₃形态较其它两者具有更好的除浊、除腐殖酸和脱色效果并且具有更强的电中和能力,因此Al₁₃形态是一种具有较高正电荷和较高的水解稳定性,在给水和废水处理中的一种较为有效的Al形态.     

铝盐混凝剂的混凝效果与残留铝含量和组分之间的关系研究

研究了氯化铝、硫酸铝、聚合氯化铝(poly-aluminum chloride, PAC)3种铝盐混凝剂在腐殖酸-高岭土模拟水样中的应用,以比较3种混凝剂在该水样中的混凝效果与残留铝含量和组分之间的关系.结果表明, 3种铝盐混凝剂在试验选取的投加量下对浊度和UV254的去除率最高可达90%左右,PAC能在较高的投加量下达到较好的混凝效果;较高投加量下PAC混凝沉淀出水中残留总铝含量为0.9 mg/L左右,余铝率为-3.0%左右,均明显低于传统的铝盐混凝剂;3种混凝剂混凝处理腐殖酸-高岭土模拟水样时,残留铝均大部分以溶解性总铝的形式存在,且溶解性有机铝在总溶解性铝中所占比例较大;PAC在腐殖酸-高岭土混凝沉淀出水中残留总铝的含量下降最快,且能够有效降低出水中毒性较大的溶解性铝的含量,其混凝沉淀出水中残留总溶解性铝含量为0.6 mg/L左右.     

纳米Al13的分离方法及混凝效果动态过程的研究

以相同Al13含量、不同浓度的PAC为原料,利用乙醇-丙酮混合溶剂法、SO4^2-／Ba^2 沉淀置换法以及柱层析法分离提纯纳米Al13形态,同时利用Al-Ferron逐时络合比色法、^27Al-NMR等多种现代分析手段进行分析鉴定,比较其分离效果,并采用烧杯实验法和透光率脉动检测技术对Al13形态以及PAC、AlCl3的絮凝效果及絮凝过程中絮集物形成和增长的变化差异作了对比性研究．实验结果表明,乙醇．丙酮混合溶剂法对Al13分离纯化效果最好,分离所得Al13平均粒径大,聚合程度高．柱层析法受柱体积的影响只对低浓度的PAC有较好的分离效果;SO4^2-／Ba^2 沉淀置换法虽具有较好的分离效果,但分离过程有其他杂质离子的加入,影响到产品品质．混凝效果和动态实验结果表明,Al13形态是在絮凝过程中起电中和作用的主要形态,具有较强的除浊及脱色能力,在混凝过程中当絮体受到剪切力的破坏时Al13形态比PAC和AlCl3具有更强重新絮凝的能力．     

Analysis and prediction of the influence of energy utilization on air quality in Beijing

This work evaluates the influence of energy consumption on the future air quality in Beijing, using 2000 as the base year and 2008 as the target year. It establishes the emission inventory of primary PM₁₀, SO₂ and NO_x related to energy utilization in eight areas of Beijing. The air quality model was adopted to simulate the temporal and spatial distribution of each pollutant concentration in the eight urban areas. Their emission, concentration distribution, and sectoral share responsibility rate were analyzed, and air quality in 2008 was predicted. The industrial sector contributed above 40% of primary PM₁₀ and SO₂ resulting from energy consumption, while vehicles accounted for about 65% of NO_x. According to the current policy and development trend, air quality in the eight urban areas could become better in 2008 when the average concentrations of primary PM₁₀, SO₂ and NO₂ related to energy utilization at each monitored site are predicted to be about 25, 50 and 51 μg/m³, respectively. Translated from China Environmental Science, 2005, 25(6): 746–750 [译自: 中国环境科学]     

Observation of black carbon aerosol in Beijing,2003

The objective of this study was to determine the black carbon concentration in Beijing in 2003. The aerosol properties were measured using an Aethalometer and a tapered element oscillating microbalance (TEOM) on the roof of the Physics Building of Peking University (39.99° N, 116.31° E) from July to August 2003 and from November 2003 to January 2004. The average black carbon (BC) concentrations in the summer and winter were 8.80 and 11.4 μg/m³, respectively. During winter, two different cyclone cut offs were installed at the inlet of an aethalometer. The BC mass concentration in TSP, PM₁₀, and PM_2.5 were obtained. The results indicated that in winter aerosol, 90% of BC exited in PM₁₀ and 82.6% of BC exited in PM_2.5. The BC in PM₁₀ accounted for 5.11% of the PM₁₀ mass. Translated from Acta Scientiae Circumstantiae, 2005, 25(1): 17–22 [译自: 环境科学学报]     

水体环境内毒素活性的鲎法定量检测及影响因素研究

内毒素是革兰氏阴性菌和某些蓝藻细胞壁上的脂多糖复合物,是常见的外源性致热原,具有强免疫刺激能力,与人类多种疾病密切相关.本研究采用最低检测限为0.03 EU.mL-1的动态浊度东方鲎(Tachypleus Amebocyte Lysate,TAL)试剂,对不同水体环境样品的内毒素活性定量检测,分析了pH值和无机盐对TAL试验检测结果的影响.结果表明pH值在6.0～8.4范围内适合进行内毒素检测,过酸条件引起检测结果的抑制,过碱条件引起检测结果的增强,检测前可用无热原Tris-HCl(pH=7.4)溶液调节pH.当NaCl、Na2SO4、CaCl2、MgCl2和KCl浓度小于50 mg.L-1时不会干扰内毒素的检测,当浓度升高至1 000～10 000 mg.L-1时引起抑制效果.浓度为2.5 mg.L-1的FeCl3、Fe2(SO4)3、AlCl3和Al2(SO4)3即可以引起强烈抑制效果,内毒素活性的实测值已经严重偏离实际值.采用动态浊度TAL试验检测超纯水、自来水和景观用水的内毒素活性,结果表明所检测的超纯水的内毒素活性<0.06 EU.mL-1,自来水的内毒素活性为0.46 EU.mL-1,景观用水的内毒素活性为432.68EU·mL-1.     

聚合氯化铝中纳米Al13形态的分离纯化及形态表征

采用超滤法和层析法分离纯化聚合氯化铝(PAC)中的Al₁₃形态,并采用Al-Ferron逐时络合比色法、²⁷Al-NMR、TEM和粒度测定仪对分离纯化所得的Al₁₃形态进行了分析和表征.研究结果表明,超滤法分离纯化的效果受超滤膜的孔径及PAC浓度的影响,选择合适孔径的膜和PAC溶液浓度即可以获得高纯度的Al₁₃,在层析法中则随着洗脱时间延长按分子的大小依次洗脱下来,因此截取中间组分即可得到Al₁₃;Al-Ferron逐时络合比色法和²⁷Al-NMR的分析结果表明,采用上述2种方法分离提纯得到的样品中Al₁₃的含量分别可达到90%以上和100%.TEM和粒度测定结果表明,在B=2.5的PAC溶液中,Al₁₃极少以Al₁₂AlO₄(OH)₂₄(H₂O)⁷⁺₁₂的单体形态存在,而是呈两维结构的线性和枝状的聚集体,Al₁₂AlO₄(OH)₂₄(H₂O)⁷⁺₁₂的聚集体尺寸通常在几十至几百nm.     

Catalytic activity of cerium-doped Ru/Al2O3 during ozonation of dimethyl phthalate

In this paper, factors influencing the mineralization of dimethyl phthalate (DMP) during catalytic ozonation with a cerium-doped Ru/Al₂O₃ catalyst were studied. The catalytic contribution was calculated through the results of a comparison experiment. It showed that doping cerium significantly enhanced catalytic activity. The total organic carbon (TOC) removal over the doped catalyst at 100 min reached 75.1%, 61.3% using Ru/Al₂O₃ catalyst and only 14.0% using ozone alone. Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto Al₂O₃ support. Results of experiments on oxidation by ozone alone, adsorption of the catalyst, Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%, which showed the obvious effect of Ru-Ce/Al₂O₃ on catalytic activity. __________ Translated from China Environmental Science, 2006, 26(4): 445–448 [译自: 中国环境科学]     

Co3O4/BiVO4复合阳极活化过一硫酸盐强化光电催化降解双酚A

采用静电纺丝法制备了Co_3O_4/BiVO_4复合薄膜电极,并以之为光阳极,在过一硫酸盐(PMS)辅助作用下开展了光电催化降解双酚A研究.结果表明,PMS在可见光下可显著强化Co_3O_4/BiVO_4复合阳极光电催化降解双酚A,在0.25 V外加偏压以及可见光照射下,当加入2 mmol·L-1PMS时,双酚A在2 h内的降解效率为96%.降解动力学常数为0.471 4 min-1.系统研究了PMS初始浓度、外加偏压对双酚A降解性能的影响.结果发现,双酚A在较低的PMS投加量和较低的外加偏压(0.25 V)下即可有效降解.采用电子自旋共振波谱仪鉴定体系的主要活性自由基为SO·-4和·OH.并进一步通过淬灭实验结果证明空穴、SO·-4和·OH起主要氧化作用.光电反应后的体系中未检测到金属离子溶出,可避免二次污染.     

信号分子强化改性挂膜沸石持续抑制沉积物中氨氮释放

为寻找一种长期有效的底泥修复方式,对沸石进行了改性并挂膜的实验.考察了 4种铝盐[AlCl3、Al(NO3)3、Al2(SO4)3和KAl(SO4)2]改性挂膜沸石对上覆水中氨氮的去除情况.结果表明,AlCl3改性挂膜沸石效果最佳,且最佳改性浓度为0.8 mol·L-1.进一步分析添加信号分子OHHL后,AlCl3改性...     

电晕放电与络合催化联合同时去除烟气中SO_2、NO实验研究

采用电晕放电与液相络合催化协同同时去除烟气中SO2和NO,电压、水流量、乙二胺合钴浓度、pH、SO2和NO初始浓度以及气流量对同时去除SO2和NO效率的影响进行了实验研究.结果表明:NO去除率随着放电电压、水流量、乙二胺合钴浓度、pH的增加而增加,而随SO2和NO初始浓度、烟气流量的增大而减小;SO2去除率也随放电电压,水流量的增加而增加,随烟气流量的增加而下降,但溶液pH,SO2和NO初始浓度和乙二胺合钴浓度对其影响很小.溶液中加入Mn2+和尿素能分别增强SO2和NO的去除效果.最佳条件为:电压25 kV、水流量80 L·h-1,乙二胺合钴浓度0.02 mol·L-1,烟气流量1.0 m3·h-1、尿素浓度0.02 mol·L-1,Mn2+浓度为0.02 mol·L-1时,NO和SO2去除率分别可达68%和94%,对应能量消耗分别为22.2 g·k Wh-1和75.2 g·k Wh-1.     

不同铝形态去除水中腐殖酸的混凝特性

制备了碱化度为2.4、以Al13,为主要成分的聚合铝PAC-All13和碱化度为2.4、以Al30为主要成分的高聚聚合铝PAC-Al30.采用烧杯混凝实验,通过絮体颗粒生长、电中和能力、pH和混凝剂投量对混凝效果的影响,比较了PAC-Al30、PAC-Al13,和AIC3,混凝去除水中腐殖酸的行为,并考察了水中残留铝的含量.实验结果表明,3种混凝剂的絮体形成能力由强到弱为PAC-Al30>PAC-Al13>AlCl3.与AlCl3相比, PAC-Al13和PAC-Al30的适用pH范围更宽,为5.0～8.0.PAC-Al30和PAC-Al13,的电中和能力差别不明显;由于更强的吸附和架桥作用,在低投量下PAC-Al30表现出更好的混凝效果,而且PAC-Al30比AlCl3和PAC-Al13有更宽的有效投量范围,为0.08～0.64mmol/L.对于腐殖酸含量为10m/L的水样,在pH为7.0,投量为0.16mmol/L下, PAC-Al30对腐殖酸去除率达到98.5%,此时出水残留铝浓度为0.066mg/L.结果证实Al30是可用于水中腐殖酸去除的一种新型的混凝/絮凝活性成.     

生活垃圾焚烧厂渗滤液生化出水的混凝机理研究

分别采用Al₂(SO₄)₃、FeCl₃、PAC、PAFC对垃圾焚烧厂渗滤液生化出水进行混凝研究,并建立混凝处理模型.结果表明,在pH值为6时,单独投加500 mg/L的Al₂(SO₄)₃、FeCl₃、PAC、PAFC时,COD去除率分别为20％、17％、30％、40％.焚烧厂渗滤液生化出水中有机物主要是由相对分子质量小于2 000的可溶性物质组成;通过透射电镜扫描技术(TEM)和Zeta电位分析,发现中和及网捕桥联是渗滤液混凝处理的主要作用机理;相比无机盐混凝剂,聚合物混凝剂具有较强的电中和以及网捕架桥功能.     

南京北郊冬春季大气能见度影响因子贡献研究

为研究南京北郊气象要素以及气溶胶对大气能见度的影响,利用2014年1~5月的能见度、相对湿度、温度、颗粒物浓度及其化学成分等观测数据,探讨了气溶胶不同化学组分对消光系数的贡献,提出了该地区能见度基于不同参数的拟合方案.结果表明,观测期间平均能见度为(5.78±3.64)km,能见度与相对湿度、PM_(2.5)存在明显的负相关,相关系数分别为-0.66、-0.48.冬季平均消光系数为(398.72±219.88)Mm~(-1),Organic、NH_4NO_3、(NH_4)_2SO_4和EC对消光的贡献率分别为38.81%、27.81%、23.95%和7.15%;春季平均消光系数为(248.36±78.42)Mm~(-1),Orgamic、NH_4NO_3、(NH_4)_2SO_4和EC对消光的贡献率分别为31.59%、24.36%、32.63%和8.64%.对比不同的能见度拟合方案时,基于颗粒物成分的能见度拟合方案优于基于散射系数的.不同相对湿度区间内PM_(2.5)对能见度的影响程度不同,基于PM_(2.5)、相对湿度和温度的能见度拟合方案说明:低相对湿度的条件下,PM_(2.5)对能见度的影响较大;随相对湿度增大,相对湿度成为更为重要的影响因子.     

烟花爆竹集中燃放的大气细颗粒物(PM2.5)成分图谱

烟花爆竹燃放是大气细颗粒物（PM_2.5）来源的途径之一.以泉州城区春节期间为例,研究烟花爆竹燃放对大气细颗粒物的影响,服务大气污染的特殊污染源管理.结果表明,烟花爆竹集中燃放时段,SO₂、PM₁₀和PM_2.5浓度明显升高,尤以PM_2.5的升高最为显著,城区PM_2.5日均浓度峰值约为年均值的4倍,涂山街点位PM_2.5小时浓度峰值约为城区年均值的21倍;燃放高峰期Al、Mg、Ba、Cu、Sr等烟花爆竹的特征元素占比迅速上升,Al⁺、Mg⁺、Ba⁺、Cu⁺间的小时数浓度高度相关;监测期间泉州城区细颗粒物主要污染源是烟花爆竹燃放和生物质燃烧,贡献占总颗粒物的一半以上,燃煤和工业工艺源的比例相对较低,均低于10.0%;集中燃放时段大气细颗粒物浓度高达0.578 mg·m^-3,此时的烟花源的贡献比例也提升到58.2%;污染过程分析表明PM_2.5浓度与烟花源的占比、数浓度的变化趋势具有趋同性.以上结果说明烟花爆竹的集中燃放是春节期间泉州大气环境恶化的主要原因.     

二氧化硫暴露对谷子幼苗气孔运动、脯氨酸代谢和抗氧化酶系统的影响

二氧化硫(SO_2)是一种有毒的大气污染物,主要经气孔进入植物体内.目前对于SO_2毒性的研究多集中在氧化损伤方面,关于SO_2对植物脯氨酸代谢的影响及相关分子机制的研究还很少.本文以谷子幼苗为材料,研究了不同浓度SO_2气体暴露对叶片气孔运动、脯氨酸代谢和抗氧化酶系统的影响.结果显示,10 mg·m~(-3) SO_2熏气对谷子幼苗的叶片形态、相对含水量、气孔开度、脯氨酸含量及抗氧化酶活性均无明显影响.30 mg·m~(-3) SO_2暴露24～72 h后,叶片出现明显的受损症状,相对含水量降低,叶面气孔开度减小;30 mg·m~(-3) SO_2熏气导致叶中脯氨酸含量显著增加,脯氨酸脱氢酶(PDH)活性明显升高.同时,长时间的SO_2胁迫可诱导SiPDH基因表达上调,而脯氨酸合成相关基因SiP5CS、SiP5CR表达受到明显抑制.此外,谷子幼苗暴露于30 mg·m~(-3) SO_2时,叶中超氧阴离子(O■)产生速率与对照相比显著提高,诱导超氧化物歧化酶(SOD)和过氧化氢酶(CAT)活性增强,从而将过氧化氢(H_2O_2)含量维持在正常水平.以上结果表明,SO_2对谷子的毒性效应具有浓度依赖性.高浓度SO_2暴露下,谷子能够通过控制气孔开放、调节脯氨酸代谢和抗氧化酶活性等过程来适应SO_2胁迫.     

水解聚合铝溶液中形态分布的定量模拟研究

通过Ａｌ－Ｆｅｒｒｏｎ逐时络合比色法和￣（２７）Ａｌ核磁共振（ＮＭＲ）法，并应用“ＭＩＮＥＱＬ”化学平衡模式计算法，对采用不同反应途径制得的聚合铝（ＰＡＣ）溶液中的化学形态分布规律进行了定量模拟研究和对比。模式计算结果与两种实验定量分析结果都较为吻合，结果表明，在水解聚合铝溶液中较稳定的化学形态主要有五种：一种单体形态［ａｌ＿ａ］，即Ａｌ￣（３＋），Ａｌ（ＯＨ）￣（２＋），Ａｌ（ＯＨ）＿２￣＋；３种聚合形态［Ａｌ＿ｂ］，即和以及一种溶胶或凝胶形态［Ａｌ＿ｃ］，即Ａｌ（ＯＨ）＿３（ａｍ）．这些化学形态的分布和转化不仅取决于溶液的化学特征，而且也取决于制备方法的不同。     

Characteristics of mass distributions of aerosol particle and its inorganic water-soluble ions in summer over a suburb farmland in Beijing

Agricultural activity is one of the most important sources of aerosol particles. To understand the mass distribution and sources of aerosol particles and their inorganic water-soluble ions in a suburb farmland of Beijing, particle samples were collected using a microorifice uniform deposit impactor (MOUDI) in the summer of 2004 in a suburb vegetable field. The distribution of the particles and their inorganic water-soluble ions in the diameter range of 0.18–18 μm were measured. The dominant fine particle ions were SO₄ ²⁻, NO₃ ⁻, and NH₄ ⁺. The association of day-to-day variation of the concentration of these ions with temperature, humidity, and solar radiation suggested that they are formed by the reaction of NH₃ released from the vegetable field with the acid species produced from photochemical reactions. Fine particle K⁺ is likely from vegetation emission and biomass burning. Coarse particles like Ca²⁺, Mg²⁺, NO₃ ⁻, and SO₄ ²⁻ are suggested to come from the mechanical process by which the soil particle entered the atmosphere, and from the reaction of the acid species at the surface of the soil particle. The results show that fertilizer and soil are important factors determining the aerosol particle over agricultural fields, and vegetable fields in suburban Beijing contribute significantly to the aerosol particle. Translated from Environmental Science, 2006, 27(2): 193–199 [译自: 环境科学]     

SO2诱导的萱草保卫细胞凋亡及其信号调节

SO2是一种常见的大气污染物,急性和慢性暴露都会对植物造成伤害.因此,本文以景观绿化植物萱草叶片下表皮为材料,研究了SO2对气孔保卫细胞的致死效应及其可能的信号调节途径.结果表明,利用SO2体内衍生物-亚硫酸钠和亚硫酸氢钠混合液处理萱草表皮3 h后,随着处理浓度(1.0~5.0 mmol·L-1)的增加,萱草保卫细胞生理活性下降,甚至死亡;浓度超过2.0 mmol·L-1时,细胞死亡率显著增高(p0.05),死细胞出现核固缩、核拉长、核碎片等典型凋亡特征,保卫细胞内的活性氧种(ROS)、一氧化氮(NO)和Ca2+水平显著升高.采用不同浓度的抗氧化剂过氧化氢酶(CAT)、抗坏血酸(AsA),Ca2+螯合剂乙二醇双四乙酸(EGTA)和Ca2+通道抑制剂氯化镧(LaCl3)及NO清除剂羧基-2苯-4,4,5,5-四甲基咪唑-1-氧-3氧化物(C-PTIO)和合成抑制剂叠氮钠(NaN3)处理后,均可使SO2衍生物诱发的细胞死亡率降低,以200 U·mL-1CAT、0.05 mmol·L-1的AsA、EGTA、LaCl3及0.20 mmol·L-1的C-PTIO、NaN3的效果最佳,同时胞内ROS、NO和Ca2+水平下降.以上结果表明,一定浓度的SO2可诱导萱草保卫细胞死亡,可能通过诱导ROS和NO爆发,激活细胞质膜钙通道,进而引起胞内Ca2+增加,通过ROS-NO-Ca2+信号途径介导细胞死亡.SO2诱导的萱草细胞死亡可能存在细胞凋亡过程.