酸碱、高温改性13X分子筛及其对苯乙烯的吸附

针对原样13X分子筛吸附速率和吸附容量低的问题,通过碱溶液(NaOH,NH_3)和酸溶液(CH_3COOH,HCl)对13X分子筛进行浸渍改性,并对酸改性后的分子筛进行高温二次处理,考察了试剂种类、试剂浓度、浸渍时间、焙烧温度、焙烧时间5个因素对分子筛吸附性能的影响,并采用SEM和BET进行了表征。结果表明:最佳改性条件是盐酸浓度6.0 mol·L~(-1)、浸渍时间24 h、焙烧温度450℃、焙烧时间6 h;在最佳条件下制备的改性分子筛极大提高了对苯乙烯的吸附速率和吸附容量;改性后的分子筛对苯乙烯的动态吸附更符合准2级动力学模型,R2均大于0.98;SEM表征结果说明改性后分子筛表面孔隙率明显增加;BET比表面积分析结果说明酸改性可使分子筛各类孔面积增加,而高温改性会使BET比表面积和中孔面积增加,微孔面积降低;相关分析结果显示,改性分子筛对苯乙烯动态饱和吸附量与BET比表面积和中孔面积均呈显著正相关。     

以粉煤灰为原料制备高纯度NaP型分子筛

以工业固体废弃物粉煤灰为原料,经分级处理后提取其中的硅铝元素(Na_2SiO_3和NaAlO_2),通过水热合成法制备高纯度NaP型分子筛。考察了硅铝比、水硅比、晶化时间和晶化温度对NaP型分子筛制备的影响,采用XRD、SEM、FTIR和DTA-TG对NaP型分子筛的晶型、形貌、热稳定性进行分析表征,并考察了NaP分子筛对Cu~(2+)的吸附性能。实验结果表明,当H_2O/Si为120、Si/Al为1.0,晶化温度为115℃、晶化时间9h时,可得到高纯度NaP型分子筛。合成的NaP型分子筛可有效地吸附Cu~(2+),温度升高有助于分子筛吸附能力的提升,当吸附温度为45℃,吸附120min时,Cu~(2+)的最大去除率可达98.3%。     

不同硅铝比的ZSM-5型沸石分子筛吸附水中Cu2＋离子的研究

考察了3种不同硅铝比的ZSM-5沸石分子筛（25H、38H和50H，25、38和50为硅铝比）对水中Cu2＋的吸附过程及其影响因素。结果表明，3种材料均能有效吸附去除水中Cu2＋离子，动力学符合假二阶动力学模型，吸附等温线符合Langmuir吸附等温式。3种材料吸附速率及吸附容量顺序为：25H〉50H〉38H，其中，25H最大吸附容量达到12．83mg／g。投加量由0．8g／L增加至2．0g／L，材料对Cu2＋吸附去除率由87．0％增加至97．5％。考察水中常见阳离子对吸附的干扰作用，结果表明，干扰离子的影响顺序为：Pb2＋〉K＋〉Na＋〉Mg2＋；随着干扰离子浓度的增大，材料对Cu2＋的去除率显著下降。硅铝比及晶粒形貌均对沸石分子筛吸附Cu2＋有较大影响，小的孔径不利于Cu2＋的吸附，低硅铝比有利于Cu2＋在分子筛上的吸附。     

分子筛吸附——低温等离子体氧化去除甲苯

利用分子筛吸附—低温等离子体氧化工艺去除甲苯,比较了HY、13X、ZSM-5 3种不同分子筛的性能、处理效果及副产物。结果表明:3种分子筛的BET比表面积、穿透吸附量和饱和吸附量均表现为HY13XZSM-5;3种分子筛用于分子筛吸附—低温等离子体氧化均能100%去除甲苯,但最终的碳平衡和CO_2选择性以HY为分子筛时最好,以ZSM-5为分子筛时最差;ZSM-5分子筛条件下产生的副产物O_3和N_2O均最多,而HY分子筛条件下产生的副产物O_3和N_2O均最少。因此,对于分子筛吸附—低温等离子体氧化去除甲苯而言,HY作为分子筛时效果最佳,而ZSM-5作为分子筛时效果最差。     

不同硅铝比的ZSM-5型沸石分子筛吸附水中Cu2+离子的研究

考察了3种不同硅铝比的ZSM-5沸石分子筛（25H、38H和50H，25、38和50为硅铝比）对水中Cu²⁺的吸附过程及其影响因素。结果表明，3种材料均能有效吸附去除水中Cu²⁺离子，动力学符合假二阶动力学模型，吸附等温线符合Langmuir吸附等温式。3种材料吸附速率及吸附容量顺序为：25H＞50H＞38H，其中，25H最大吸附容量达到12.83 mg/g。投加量由0.8 g/L增加至2.0 g/L，材料对Cu²⁺吸附去除率由87.0%增加至97.5%。考察水中常见阳离子对吸附的干扰作用，结果表明，干扰离子的影响顺序为：Pb²⁺> K⁺> Na⁺ > Mg²⁺；随着干扰离子浓度的增大，材料对Cu²⁺的去除率显著下降。硅铝比及晶粒形貌均对沸石分子筛吸附Cu2+有较大影响，小的孔径不利于Cu²⁺的吸附，低硅铝比有利于Cu²⁺在分子筛上的吸附。     

中孔分子筛Al-MCM-41催化裂解聚烯烃反应研究

采用水热合成法制备了不同硅铝比的中孔分子筛A l-MCM-41,将其应用于高密度聚乙烯(HDPE)和聚丙烯(PP)的催化裂解反应。通过改变硅铝比、反应温度和催化剂用量,对A l-MCM-41催化HDPE和PP裂解反应的规律进行了探讨,研究表明,HDPE裂解反应受硅铝比的影响较大;而对于PP裂解反应,硅铝比在一定范围内对催化剂活性的影响不明显。另外,与热裂解和HZSM-5小孔分子筛的催化裂解结果进行了比较,结果证明A l-MCM-41具有较高的催化活性和较高的液体产物收率,尤其适合于空间位阻较大的PP的催化裂解反应。     

用煤矸石合成4A沸石分子筛处理氨氮废水

以煤矸石为原料，采用碱熔一水热法合成4A沸石分子筛。由于煤矸石中铝、硅主要以高岭土形式存在，其活化过程是合成4A沸石分子筛关键环节。为提高4A沸石分子筛钙离子的交换能力，增加对模拟废水氨氮的去除率，实验考察了碳酸钠与煤矸石质量比、活化温度、活化时间、晶化温度和晶化时间对4A沸石分子筛钙离子交换能力的影响，同时也考察了模拟废水的pH、4A沸石分子筛加入量及吸附时间对氨氮去除率的影响。结果表明，最佳工艺条件为，碳酸钠与煤矸石质量比为0．9、活化温度为800％、活化时间1．5h、晶化温度90％和晶化时间3h。合成4A沸石分子筛的钙离子交换能力为310mg／g，在pH为6的100mL模拟氨氮废水中加入6g4A沸石分子筛吸附40min后，废水中氨氮的去除率达到86％。通过最佳工艺条件合成4A沸石分子筛，在处理氨氮废水方面具有一定的应用前景。     

用煤矸石合成4A沸石分子筛处理氨氮废水

以煤矸石为原料,采用碱熔-水热法合成4A沸石分子筛。由于煤矸石中铝、硅主要以高岭土形式存在,其活化过程是合成4A沸石分子筛关键环节。为提高4A沸石分子筛钙离子的交换能力,增加对模拟废水氨氮的去除率,实验考察了碳酸钠与煤矸石质量比、活化温度、活化时间、晶化温度和晶化时间对4A沸石分子筛钙离子交换能力的影响,同时也考察了模拟废水的pH、4A沸石分子筛加入量及吸附时间对氨氮去除率的影响。结果表明,最佳工艺条件为,碳酸钠与煤矸石质量比为0.9、活化温度为800℃、活化时间1.5 h、晶化温度90℃和晶化时间3 h。合成4A沸石分子筛的钙离子交换能力为310 mg/g,在pH为6的100 mL模拟氨氮废水中加入6 g 4A沸石分子筛吸附40 min后,废水中氨氮的去除率达到86%。通过最佳工艺条件合成4A沸石分子筛,在处理氨氮废水方面具有一定的应用前景。     

用稻壳硅源水热合成P型分子筛的研究

利用稻壳中丰富的氧化硅为硅源,以Al(OH)3为外加铝源,采用水热法合成P型分子筛.通过实验得到制备P型分子筛的最佳条件:硅铝摩尔比(SiO2/A12O3)为5.6,钠硅摩尔比(Na2O/SiO2)为1.43,水钠摩尔比(H2O/Na2O)为18.3,反应温度为85℃,反应时间为24 h.X射线衍射(XRD)与扫描电镜...     

中孔分子筛AI-MCM-41催化裂解聚烯烃反应研究

采用水热合成法制备了不同硅铝比的中孔分子筛AI-MCM-41，将其应用于高密度聚乙烯（HDPE）和聚丙烯（PP）的催化裂解反应。通过改变硅铝比、反应温度和催化剂用量，对Al-MCM-41催化HDPE和PP裂解反应的规律进行了探讨，研究表明，HDPE裂解反应受硅铝比的影响较大；而对于PP裂解反应，硅铝比在一定范围内对催化剂活性的影响不明显。另外，与热裂解和HZSM-5小孔分子筛的催化裂解结果进行了比较，结果证明A1-MCM-41具有较高的催化活性和较高的液体产物收率，尤其适合于空间位阻较大的PP的催化裂解反应。     

Air-Surface Exchange of Mercury with Soils Amended with Ash Materials

Abstract

Air-surface exchange of mercury (Hg) was measured from soil low in Hg (0.013 mg/kg) amended with four different ash materials: a wood ash containing ～10% coal ash (0.070 mg/kg Hg), a mixture of two subbituminous coal fly ashes (0.075 mg/kg Hg), a subbituminous coal ash containing ～10% petroleum coke ash (1.2 mg/kg Hg), and an ash from incinerated municipal sewage sludge (4.3 mg/kg Hg) using a dynamic flux chamber. Ash was added to soil to simulate agricultural supplements, soil stabilization, and pad layers used in livestock areas. For the agricultural amendment, ～0.4% ash was well mixed into the soil. To make the stabilized soil that could be used for construction purposes, ～20% ash was mixed into soil with water. The pad layer consisted of a wetted 1-cm layer of ash material on the soil surface. Diel trends of Hg flux were observed for all of the substrates with significantly higher Hg emissions during the day and negligible flux or deposition of Hg during the night. Hg fluxes, which were measured in the summer months, were best correlated with solar radiation, temperature, and air O₃ concentrations. Mean Hg fluxes measured outdoors for unamended soils ranged from 19 to 140 ng/m² day, whereas those for soil amended with ash to simulate an agricultural application ranged from 7.2 to 230 ng/m² day. Fluxes for soil stabilized with ash ranged from 77 to 530 ng/m² day and for soil with pads constructed of ash ranged from ?50 to 90 ng/m² day. Simple analytical tests (i.e., total Hg content, synthetic precipitation leaching procedure, heating, and indoor gas-exchange experiments) were performed to assess whether algorithms based on these tests could be used to predict Hg fluxes observed outdoors using the flux chamber. Based on this study, no consistent relationships could be developed. More work is needed to assess long-term and seasonal variations in Hg flux from (intact and disturbed) substrates before annual estimates of emissions can be developed.     

Air-surface exchange of mercury with soils amended with ash materials

Air-surface exchange of mercury (Hg) was measured from soil low in Hg (0.013 mg/kg) amended with four different ash materials: a wood ash containing -10% coal ash (0.070 mg/kg Hg), a mixture of two subbituminous coal fly ashes (0.075 mg/kg Hg), a subbituminous coal ash containing -10% petroleum coke ash (1.2 mg/kg Hg), and an ash from incinerated municipal sewage sludge (4.3 mg/kg Hg) using a dynamic flux chamber. Ash was added to soil to simulate agricultural supplements, soil stabilization, and pad layers used in livestock areas. For the agricultural amendment, -0.4% ash was well mixed into the soil. To make the stabilized soil that could be used for construction purposes, -20% ash was mixed into soil with water. The pad layer consisted of a wetted 1-cm layer of ash material on the soil surface. Diel trends of Hg flux were observed for all of the substrates with significantly higher Hg emissions during the day and negligible flux or deposition of Hg during the night. Hg fluxes, which were measured in the summer months, were best correlated with solar radiation, temperature, and air O3 concentrations. Mean Hg fluxes measured outdoors for unamended soils ranged from 19 to 140 ng/m2 day, whereas those for soil amended with ash to simulate an agricultural application ranged from 7.2 to 230 ng/m2 day. Fluxes for soil stabilized with ash ranged from 77 to 530 ng/m2 day and for soil with pads constructed of ash ranged from -50 to 90 ng/m2 day. Simple analytical tests (i.e., total Hg content, synthetic precipitation leaching procedure, heating, and indoor gas-exchange experiments) were performed to assess whether algorithms based on these tests could be used to predict Hg fluxes observed outdoors using the flux chamber. Based on this study, no consistent relationships could be developed. More work is needed to assess long-term and seasonal variations in Hg flux from (intact and disturbed) substrates before annual estimates of emissions can be developed.     

Co-inoculation with beneficial microorganisms enhances tannery sludge bioleaching with Acidithiobacillus thiooxidans

Environmental Science and Pollution Research - Bioleaching of tannery sludge is an efficient and environmentally friendly way for chromium (Cr) removal, which supports the sustainable development...     

Advances with supercritical fluids

In the last decade, supercritical fluids more and more have been proved as environmentally benign media for chemical and related processes. Many new processes and products have been developed, using the inherent physical and chemical properties of supercritical fluids. Moreover, these processes also promise economic effects. The prerequisites for this success however, are a sound knowledge of physico-chemical properties of--and phenomena in--supercritical mixtures and the availability of other chemical engineering data. This requires an effective exchange of knowledge between a large number of branches of science. In the following, a lot of recent papers will be cited, which should give an overview of actual results on fundamentals and their applications.     

Evolution of clog formation with time in columns permeated with synthetic landfill leachate

Laboratory column tests conducted to gain insight regarding the biological and chemical clogging mechanisms in a porous medium are presented. To seed the porous medium with landfill bacteria, a mixture of Keele Valley Landfill and synthetic leachate permeated through the column under anaerobic conditions for the first 9 days of operation. After this, 100% synthetic leachate was used. The synthetic leachate approximated Keele Valley Landfill leachate in chemical composition but contained negligible suspended solids and bacteria compared with real leachate. The removal of volatile fatty acids (VFAs), primarily acetate, in leachate as it passed through the medium was highly correlated with the precipitation of calcium carbonate (CaCO(3(s))) from solution. The columns experienced a decrease in drainable porosity from an initial value of about 0.38 to less than 0.1 after steady state chemical oxygen demand (COD) removal, resulting in a five-order magnitude decrease in hydraulic conductivity. The decrease in drainable porosity prior to steady state COD removal was primarily due to the growth of a biofilm on the medium surface. After steady state COD removal, calcium precipitation was at least equally responsible for the decrease in drainable porosity as biofilm growth. Clog composition analyses showed that CaCO(3(s)) was the dominant clog constituent and that 99% of the carbonate in the clog material was bound to calcium.     

Rapid treatment of water contamined with atrazine and parathion with zero-valent iron.

The utility of fine-grained iron metal in the remediation of water contamined with Atrazine and Parathion was investigated. Batch procedures under water treatment conditions (ambient temperature and pH of approximately 7) indicated that these pesticides degrade rapidly in the presence of iron powder (40-60 mesh, 40 g/l). The decline in the concentration of pesticide was monitored by HPLC. Experiments with unbuffered solutions showed a steady increase in pH values during the reactions. Therefore, experiments were run in buffered solutions. Different buffered solutions resulted in different degradation rates indicating that the buffer plays an important role in enhancing the degradation process. Tests were also performed on an industrial effluent solution containing a variety of pesticides. Although the products of degradation were not characterized, our HPLC results indicated the disappearance of all the parent pollutants.     

Phytoremediation of pyrene contaminated soils amended with compost and planted with ryegrass and alfalfa

Ryegrass (Lolium perenne) and alfalfa (Medicago sativa) were planted in pots to remediate pyrene contaminated quartz sand (as a control group), alluvial and red soils amended with and without compost. The pyrene degradation percentages in quartz sand, alluvial soil, and red soil amended with compost (5%, w/w) and planted with ryegrass and alfalfa for 90 d growth were 98-99% and 97-99%, respectively, while those of pyrene in the corresponding treatments amended without compost but planted with ryegrass and alfalfa were 91-96% and 58-89%, respectively. Further, those of pyrene in the respective treatments amended with and without compost but unplanted were 54-77% and 51-63%, respectively. Pyrene contents in both roots and aboveground parts of ryegrass and alfalfa after 90 d growth in quartz sand and the two soils amended with or without compost were trace amounts. Statistical analyses for the parameters of ryegrass planted in red and alluvial soils including the concentrations of total water-soluble volatile low molecular weight organic acids, microbial population, pyrene degradation percentage, and spiked pyrene concentration show significant correlations at 5% and mostly 1% probability levels, by the analysis of variance. It was thus suggested that the interactions among the consortia of plant root exudates, microorganisms, and amended compost in rhizosphere soils could facilitate bioavailability of pyrene and subsequently enhance its dissipation.     

Maximum ground-level concentrations with downwash--analysis

Equations derived previously for critical downwind distance xc' wind speed uc' and plume rise zc' the values that produce maximum ground-level concentrations (MGLC) chi c under downwash conditions, have been solved. Tables of chi c' xc' uc' and zc' and graphs of the relationships among uc and zc, for a range of stack heights hs' and building heights hb' are presented. Results for two types of sources--a turbine and a reciprocating engine--are discussed. Some comparisons are made to the U.S. Environmental Protection Agency's (EPA) SCREEN3 model.