碳基材料对典型PPCPs在水环境中的吸附行为研究
发布时间：2018-07-21 12:51
【摘要】：近年来,随着药品和个人护理用品(pharmaceuticals and personal care products,PPCPs)的大量使用,它们通过各种途径进入地表水、地下水及土壤等,PPCPs对环境的危害已经引起了广泛关注。三氯生是一种常用的杀菌剂,磺胺甲恶唑是一种常用的抗菌药,由于传统的污水处理方法不能有效去除PPCPs,因此在水环境中不断有此类物质检出。碳基材料(如活性炭)由于具有易操作,简单高效的特性,常被用于各类污水的处理中。但目前大部分研究仅选取了一种或者两种碳基材料作为吸附剂研究其与PPCPs的吸附行为,不同种类的碳基材料与PPCPs的吸附行为仍处于空白状态。本研究选用了三氯生和磺胺甲恶唑两种典型PPCPs作为目标污染物,选取了七种碳基材料(活性炭、椰壳炭、普通CNTs、羟基化CNTs(CNTs-OH)、羧基化CNTs(CNTs-COOH)、稻壳炭和竹炭)作为吸附剂,系统的研究了七种碳基材料与三氯生/磺胺甲恶唑的吸附行为。其中碳纳米管(carbon nanotubes,CNTs)由于具有大的比表面积、丰富孔隙结构使它具有良好的吸附性,在水处理材料领域受到很好的关注。但由于CNTs在水中容易团聚的特性,目前的研究仅限于团聚态的CNTs和部分PPCPs的吸附作用。超声是工业中分散CNTs的常用方法,但若经超声处理的CNTs释放到环境中并在环境迁移中与环境污染物结合,则CNTs和污染物的环境风险会显著增大。因此揭示CNTs的分散状态对其吸附PPCPs的影响,阐明PPCPs与分散态CNTs的吸附效果和机理有重大意义。本课题通过静态实验,主要研究了以下三个方面的内容:(1)不同碳基吸附剂(活性炭、椰壳炭、普通CNTs、CNTs-OH、CNTs-COOH、稻壳炭和竹炭)与三氯生和磺胺甲恶唑的吸附行为。通过实验结果发现,七种碳基吸附剂对三氯生和磺胺甲恶唑的吸附量均按以下顺序递减:活性炭椰壳炭普通CNTsCNTs-OHCNTs-COOH稻壳炭竹炭。同时,七种碳基吸附剂对三氯生和磺胺甲恶唑的动力学吸附过程均符合二级动力学,且七种碳基吸附剂对三氯生和磺胺甲恶唑的吸附等温线均符合Dubinin-Ashtakhov吸附模型。(2)结合不同的水化学条件研究超声对CNTs与三氯生和磺胺甲恶唑吸附行为的影响。通过实验结果可以得出,超声显著提高了三种碳纳米管的分散性,经超声处理后的不同取代基的CNTs对三氯生/磺胺甲恶唑的吸附速率和吸附量均有提高,经超声处理后的三种不同取代基的CNTs对三氯生/磺胺甲恶唑的动力学吸附和等温线吸附依然符合二级动力学和Dubinin-Ashtakhov吸附模型。离子强度对超声处理前后的不同取代基的CNTs与三氯生/磺胺甲恶唑的吸附过程有一定的影响,随离子强度的增加三氯生和磺胺甲恶唑在三种CNTs上的吸附均为先升高后降低,分别在0.035 M和0.0075 M时达到最大值。pH显著影响了超声前后的不同取代基的CNTs对三氯生/磺胺甲恶唑的吸附过程。对于三氯生来说,随着pH的升高,三种不同取代基的CNTs对三氯生的吸附量均逐渐降低;而对于磺胺甲恶唑来说,随着pH的增大,磺胺甲恶唑在三种CNTs上的吸附量先升高后降低,在pH为5时,达到最大值。这是由于在不同pH条件下三氯生和磺胺甲恶唑的表面电荷的不同。(3)研究了不同浓度的腐殖酸(Humic acid,HA)和富里酸(Fulvic acid,FA)对三种不同取代基的CNTs与同一浓度的三氯生(8 mg/L)吸附行为的影响。研究结果表明:随着HA和FA浓度的增大,CNTs对三氯生的吸附量先降低后升高,在20 mg/L时达到最小值,这可能是竞争吸附与分散作用共同作用的结果。在上述结果的基础上,选取了三个特殊浓度(0,20,200mg/L)研究固定浓度的HA和FA对CNTs和三氯生吸附等温线的影响,结果发现,对于HA来说,20mg/L的HA对吸附抑制作用最强,而与未添加HA的相比,HA为200mg/L时,在三氯生的初始浓度较低时,200mg/L的HA抑制吸附,当三氯生的初始浓度较高时,200 mg/L的HA随CNTs的吸附有促进作用。对于FA来说,20 mg/L和200 mg/L的FA均对吸附过程起抑制作用。这可能与HA和FA的特性有关。研究结果有利于进一步完善不同种类的碳基材料与三氯生/磺胺甲恶唑的吸附行为,同时进一步解释不同分散状态的CNTs对三氯生的吸附机理,为应用不同的碳基材料作为高效污水处理吸附剂提供理论支持。
[Abstract]:In recent years, with the extensive use of pharmaceuticals and personal care products (PPCPs), they have entered surface water, ground water and soil through a variety of ways. The harm of PPCPs to the environment has attracted wide attention. Three chloro Sheng is a common bactericide, sulfamethoxazole is a common antibacterial agent. Because traditional sewage treatment methods can not effectively remove PPCPs, this kind of material is constantly detected in water environment. Carbon based materials (such as activated carbon) are often used in the treatment of various kinds of sewage because of their easy to operate, simple and efficient characteristics. But at present, one or two carbon based materials are selected as adsorbents in most studies. The adsorption behavior of PPCPs and the adsorption behavior of different kinds of carbon based materials and PPCPs is still in the blank state. This study selected two typical PPCPs as target pollutants and selected seven kinds of carbon based materials (active carbon, coconut shell charcoal, common CNTs, hydroxylated CNTs (CNTs-OH), carboxylated CNTs (CNTs-COOH), rice, rice, and rice. Shell charcoal and bamboo charcoal as adsorbents, the adsorption behavior of seven carbon based materials and three chloro Sheng / sulfamethoxazole was systematically studied. The carbon nanotube (carbon nanotubes, CNTs) has a good adsorption property because of its large specific surface area and rich pore structure, which is well paid attention to in the field of water treatment materials, but because CNTs is in water. At present, the characteristics of easy reunion are limited to the adsorption of CNTs and partial PPCPs in the reunion state. Ultrasound is a common method for dispersing CNTs in industry. However, the environmental risk of CNTs and contaminants will be significantly increased if the CNTs treated by ultrasound is released into the environment and is combined with environmental pollutants in environmental migration. Thus, CNTs is revealed. The influence of the dispersion state on its adsorption of PPCPs and the adsorption effect and mechanism of PPCPs and dispersed CNTs are of great significance. In this subject, the following three aspects are mainly studied through static experiments: (1) different carbon based adsorbents (active carbon, coconut shell charcoal, common CNTs, CNTs-OH, CNTs-COOH, rice hull charcoal and bamboo charcoal) and three chloro and sulfonamides The adsorption behavior of oxazoxazole shows that the adsorption of seven carbon based adsorbents on three chloro and sulfamethoxazole is decreasing in the following order: activated carbon coconut coconut carbon common CNTsCNTs-OHCNTs-COOH rice carbon bamboo charcoal. At the same time, the kinetic adsorption of seven carbon based adsorbents on three chloro and sulfamethoxazole conforms to the two class power. The adsorption isotherms of seven carbon based adsorbents for three chloro and sulfamethoxazole conforms to the Dubinin-Ashtakhov adsorption model. (2) the effects of ultrasound on the adsorption behavior of CNTs with three chloro and sulfamethoxazole are studied in combination with different hydrochemical conditions. Through the experimental results, the dispersion of three kinds of carbon nanotubes can be significantly increased by ultrasound. The adsorption rate and adsorption capacity of three chloro Sheng / sulfamethoxazole with different substituents after ultrasonic treatment are improved. The dynamic adsorption and isotherm adsorption of the three different substituents after ultrasonic treatment on three chloro Sheng / sulfamethoxazole and isotherm adsorption still conform to the two stage dynamics and Dubinin-Ashtakhov adsorption model. The ionic strength is strong. CNTs of different substituents before and after ultrasonic treatment has a certain influence on the adsorption process of three chloro Sheng / sulfamethoxazole. With the increase of ionic strength, the adsorption of three chloro and sulfamethoxazole on three kinds of CNTs is increased first and then decreased, and the maximum value.PH at 0.035 M and 0.0075 M, respectively, affects the different extraction before and after ultrasound. The adsorption of three chloro Sheng / sulfamethoxazole by the subgroup CNTs. For three chloropoxy, with the increase of pH, the adsorption capacity of three different substituents of CNTs to three chloro is gradually reduced; for sulfamethoxazole, with the increase of pH, the adsorption capacity of sulfonamoxazole on three kinds of CNTs increases first and then decreases, and reaches the highest level when pH is 5. Large value. This is due to the difference between the surface charge of three chloro and sulfamethoxazole under different pH conditions. (3) the effects of different concentrations of humic acid (Humic acid, HA) and rich acid (Fulvic acid, FA) on the adsorption behavior of three different substituents of CNTs and the same concentration of three chloride (8 mg/L). The results show that with HA and FA concentration In addition, the adsorption of three chlorinated three chloride increased first and then increased and reached a minimum at 20 mg/L. This may be the result of the co action of competitive adsorption and dispersion. On the basis of the above results, the effects of three special concentrations (0,20200mg/L) on the adsorption isotherms of CNTs and three chloro on the adsorption isotherms of CNTs and FA were studied. For HA, the inhibitory effect of 20mg/L's HA on adsorption is the strongest, and when HA is 200mg/L, when the initial concentration of three chloro Sheng is lower, the HA of 200mg/L is inhibited. When the initial concentration of three chloride is higher, the 200 mg/L HA is promoted with CNTs adsorption. For FA, 20 and 200 are both of the adsorption process. The results may be related to the characteristics of HA and FA. The results are beneficial to further improve the adsorption behavior of different kinds of carbon based materials and three chloro Sheng / sulfamethoxazole, and further explain the adsorption mechanism of CNTs on three chlorides in different dispersion States, and to use different carbon based materials as efficient wastewater treatment adsorbents. For theoretical support.
【学位授予单位】：北京建筑大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X703
本文编号：2135584
[Abstract]:In recent years, with the extensive use of pharmaceuticals and personal care products (PPCPs), they have entered surface water, ground water and soil through a variety of ways. The harm of PPCPs to the environment has attracted wide attention. Three chloro Sheng is a common bactericide, sulfamethoxazole is a common antibacterial agent. Because traditional sewage treatment methods can not effectively remove PPCPs, this kind of material is constantly detected in water environment. Carbon based materials (such as activated carbon) are often used in the treatment of various kinds of sewage because of their easy to operate, simple and efficient characteristics. But at present, one or two carbon based materials are selected as adsorbents in most studies. The adsorption behavior of PPCPs and the adsorption behavior of different kinds of carbon based materials and PPCPs is still in the blank state. This study selected two typical PPCPs as target pollutants and selected seven kinds of carbon based materials (active carbon, coconut shell charcoal, common CNTs, hydroxylated CNTs (CNTs-OH), carboxylated CNTs (CNTs-COOH), rice, rice, and rice. Shell charcoal and bamboo charcoal as adsorbents, the adsorption behavior of seven carbon based materials and three chloro Sheng / sulfamethoxazole was systematically studied. The carbon nanotube (carbon nanotubes, CNTs) has a good adsorption property because of its large specific surface area and rich pore structure, which is well paid attention to in the field of water treatment materials, but because CNTs is in water. At present, the characteristics of easy reunion are limited to the adsorption of CNTs and partial PPCPs in the reunion state. Ultrasound is a common method for dispersing CNTs in industry. However, the environmental risk of CNTs and contaminants will be significantly increased if the CNTs treated by ultrasound is released into the environment and is combined with environmental pollutants in environmental migration. Thus, CNTs is revealed. The influence of the dispersion state on its adsorption of PPCPs and the adsorption effect and mechanism of PPCPs and dispersed CNTs are of great significance. In this subject, the following three aspects are mainly studied through static experiments: (1) different carbon based adsorbents (active carbon, coconut shell charcoal, common CNTs, CNTs-OH, CNTs-COOH, rice hull charcoal and bamboo charcoal) and three chloro and sulfonamides The adsorption behavior of oxazoxazole shows that the adsorption of seven carbon based adsorbents on three chloro and sulfamethoxazole is decreasing in the following order: activated carbon coconut coconut carbon common CNTsCNTs-OHCNTs-COOH rice carbon bamboo charcoal. At the same time, the kinetic adsorption of seven carbon based adsorbents on three chloro and sulfamethoxazole conforms to the two class power. The adsorption isotherms of seven carbon based adsorbents for three chloro and sulfamethoxazole conforms to the Dubinin-Ashtakhov adsorption model. (2) the effects of ultrasound on the adsorption behavior of CNTs with three chloro and sulfamethoxazole are studied in combination with different hydrochemical conditions. Through the experimental results, the dispersion of three kinds of carbon nanotubes can be significantly increased by ultrasound. The adsorption rate and adsorption capacity of three chloro Sheng / sulfamethoxazole with different substituents after ultrasonic treatment are improved. The dynamic adsorption and isotherm adsorption of the three different substituents after ultrasonic treatment on three chloro Sheng / sulfamethoxazole and isotherm adsorption still conform to the two stage dynamics and Dubinin-Ashtakhov adsorption model. The ionic strength is strong. CNTs of different substituents before and after ultrasonic treatment has a certain influence on the adsorption process of three chloro Sheng / sulfamethoxazole. With the increase of ionic strength, the adsorption of three chloro and sulfamethoxazole on three kinds of CNTs is increased first and then decreased, and the maximum value.PH at 0.035 M and 0.0075 M, respectively, affects the different extraction before and after ultrasound. The adsorption of three chloro Sheng / sulfamethoxazole by the subgroup CNTs. For three chloropoxy, with the increase of pH, the adsorption capacity of three different substituents of CNTs to three chloro is gradually reduced; for sulfamethoxazole, with the increase of pH, the adsorption capacity of sulfonamoxazole on three kinds of CNTs increases first and then decreases, and reaches the highest level when pH is 5. Large value. This is due to the difference between the surface charge of three chloro and sulfamethoxazole under different pH conditions. (3) the effects of different concentrations of humic acid (Humic acid, HA) and rich acid (Fulvic acid, FA) on the adsorption behavior of three different substituents of CNTs and the same concentration of three chloride (8 mg/L). The results show that with HA and FA concentration In addition, the adsorption of three chlorinated three chloride increased first and then increased and reached a minimum at 20 mg/L. This may be the result of the co action of competitive adsorption and dispersion. On the basis of the above results, the effects of three special concentrations (0,20200mg/L) on the adsorption isotherms of CNTs and three chloro on the adsorption isotherms of CNTs and FA were studied. For HA, the inhibitory effect of 20mg/L's HA on adsorption is the strongest, and when HA is 200mg/L, when the initial concentration of three chloro Sheng is lower, the HA of 200mg/L is inhibited. When the initial concentration of three chloride is higher, the 200 mg/L HA is promoted with CNTs adsorption. For FA, 20 and 200 are both of the adsorption process. The results may be related to the characteristics of HA and FA. The results are beneficial to further improve the adsorption behavior of different kinds of carbon based materials and three chloro Sheng / sulfamethoxazole, and further explain the adsorption mechanism of CNTs on three chlorides in different dispersion States, and to use different carbon based materials as efficient wastewater treatment adsorbents. For theoretical support.
【学位授予单位】：北京建筑大学
【学位级别】：硕士
【学位授予年份】：2017
【分类号】：X703
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