碳基材料對典型PPCPs在水環(huán)境中的吸附行為研究
發(fā)布時間：2018-07-21 12:51
【摘要】：近年來,隨著藥品和個人護理用品(pharmaceuticals and personal care products,PPCPs)的大量使用,它們通過各種途徑進入地表水、地下水及土壤等,PPCPs對環(huán)境的危害已經(jīng)引起了廣泛關(guān)注。三氯生是一種常用的殺菌劑,磺胺甲惡唑是一種常用的抗菌藥,由于傳統(tǒng)的污水處理方法不能有效去除PPCPs,因此在水環(huán)境中不斷有此類物質(zhì)檢出。碳基材料(如活性炭)由于具有易操作,簡單高效的特性,常被用于各類污水的處理中。但目前大部分研究僅選取了一種或者兩種碳基材料作為吸附劑研究其與PPCPs的吸附行為,不同種類的碳基材料與PPCPs的吸附行為仍處于空白狀態(tài)。本研究選用了三氯生和磺胺甲惡唑兩種典型PPCPs作為目標污染物,選取了七種碳基材料(活性炭、椰殼炭、普通CNTs、羥基化CNTs(CNTs-OH)、羧基化CNTs(CNTs-COOH)、稻殼炭和竹炭)作為吸附劑,系統(tǒng)的研究了七種碳基材料與三氯生/磺胺甲惡唑的吸附行為。其中碳納米管(carbon nanotubes,CNTs)由于具有大的比表面積、豐富孔隙結(jié)構(gòu)使它具有良好的吸附性,在水處理材料領(lǐng)域受到很好的關(guān)注。但由于CNTs在水中容易團聚的特性,目前的研究僅限于團聚態(tài)的CNTs和部分PPCPs的吸附作用。超聲是工業(yè)中分散CNTs的常用方法,但若經(jīng)超聲處理的CNTs釋放到環(huán)境中并在環(huán)境遷移中與環(huán)境污染物結(jié)合,則CNTs和污染物的環(huán)境風險會顯著增大。因此揭示CNTs的分散狀態(tài)對其吸附PPCPs的影響,闡明PPCPs與分散態(tài)CNTs的吸附效果和機理有重大意義。本課題通過靜態(tài)實驗,主要研究了以下三個方面的內(nèi)容:(1)不同碳基吸附劑(活性炭、椰殼炭、普通CNTs、CNTs-OH、CNTs-COOH、稻殼炭和竹炭)與三氯生和磺胺甲惡唑的吸附行為。通過實驗結(jié)果發(fā)現(xiàn),七種碳基吸附劑對三氯生和磺胺甲惡唑的吸附量均按以下順序遞減:活性炭椰殼炭普通CNTsCNTs-OHCNTs-COOH稻殼炭竹炭。同時,七種碳基吸附劑對三氯生和磺胺甲惡唑的動力學吸附過程均符合二級動力學,且七種碳基吸附劑對三氯生和磺胺甲惡唑的吸附等溫線均符合Dubinin-Ashtakhov吸附模型。(2)結(jié)合不同的水化學條件研究超聲對CNTs與三氯生和磺胺甲惡唑吸附行為的影響。通過實驗結(jié)果可以得出,超聲顯著提高了三種碳納米管的分散性,經(jīng)超聲處理后的不同取代基的CNTs對三氯生/磺胺甲惡唑的吸附速率和吸附量均有提高,經(jīng)超聲處理后的三種不同取代基的CNTs對三氯生/磺胺甲惡唑的動力學吸附和等溫線吸附依然符合二級動力學和Dubinin-Ashtakhov吸附模型。離子強度對超聲處理前后的不同取代基的CNTs與三氯生/磺胺甲惡唑的吸附過程有一定的影響,隨離子強度的增加三氯生和磺胺甲惡唑在三種CNTs上的吸附均為先升高后降低,分別在0.035 M和0.0075 M時達到最大值。pH顯著影響了超聲前后的不同取代基的CNTs對三氯生/磺胺甲惡唑的吸附過程。對于三氯生來說,隨著pH的升高,三種不同取代基的CNTs對三氯生的吸附量均逐漸降低;而對于磺胺甲惡唑來說,隨著pH的增大,磺胺甲惡唑在三種CNTs上的吸附量先升高后降低,在pH為5時,達到最大值。這是由于在不同pH條件下三氯生和磺胺甲惡唑的表面電荷的不同。(3)研究了不同濃度的腐殖酸(Humic acid,HA)和富里酸(Fulvic acid,FA)對三種不同取代基的CNTs與同一濃度的三氯生(8 mg/L)吸附行為的影響。研究結(jié)果表明:隨著HA和FA濃度的增大,CNTs對三氯生的吸附量先降低后升高,在20 mg/L時達到最小值,這可能是競爭吸附與分散作用共同作用的結(jié)果。在上述結(jié)果的基礎(chǔ)上,選取了三個特殊濃度(0,20,200mg/L)研究固定濃度的HA和FA對CNTs和三氯生吸附等溫線的影響,結(jié)果發(fā)現(xiàn),對于HA來說,20mg/L的HA對吸附抑制作用最強,而與未添加HA的相比,HA為200mg/L時,在三氯生的初始濃度較低時,200mg/L的HA抑制吸附,當三氯生的初始濃度較高時,200 mg/L的HA隨CNTs的吸附有促進作用。對于FA來說,20 mg/L和200 mg/L的FA均對吸附過程起抑制作用。這可能與HA和FA的特性有關(guān)。研究結(jié)果有利于進一步完善不同種類的碳基材料與三氯生/磺胺甲惡唑的吸附行為,同時進一步解釋不同分散狀態(tài)的CNTs對三氯生的吸附機理,為應(yīng)用不同的碳基材料作為高效污水處理吸附劑提供理論支持。
[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.
【學位授予單位】：北京建筑大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X703
本文編號：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.
【學位授予單位】：北京建筑大學
【學位級別】：碩士
【學位授予年份】：2017
【分類號】：X703
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