三种典型表面活性剂在海洋沉积物上的吸附研究
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摘要
表面活性剂是常见的有机污染物,也是有机化学工业的主要原料。含表面活性剂的废水排入海洋会对生态环境、水产品安全及人类健康造成极大影响,已经引起了化学家和环境学家的广泛重视。研究沉积物对表面活性剂的吸附作用,有利于了解其在环境中的迁移转化和生物生态效应,可为控制污染提供依据。本论文的研究对象是海洋环境中广泛存在的表面活性剂类有机污染物。研究它们在海洋沉积物上的吸附行为具有重要的环境意义、生态意义和地球化学意义,因而本论文的研究成果必将为海洋环境保护和海洋科学研究提供有价值的科学依据。
本论文通过实验室模拟,研究了三种典型表面活性剂失水山梨醇聚氧乙烯(20)醚月桂酸酯(Tween20)、十二烷基苯磺酸钠(SDBS)、十六烷基三甲基溴化铵(CTAB)在海洋沉积物上的吸附行为,重点探讨了其在不同处理方式的海洋沉积物上的吸附等温线的差异及海水盐度、酸度、温度等环境因素对其吸附的影响。得到了如下结论:
A.无论在何种介质(天然海水NSW、稀释海水DSW、蒸馏水DW)中,Tween20在海洋沉积物上吸附达到平衡的时间约为50min,SDBS为100min,CTAB约为1h。吸附介质对平衡时间没有影响,但会影响沉积物对表面活性剂的吸附百分数,顺序如下:NSW>DSW>DW。
B.三种表面活性剂在HCl和水处理的沉积物上的吸附行为均可用线性吸附等温线描述,吸附主要是通过沉积物中有机碳的分配作用来完成的。SDBS在HCl和水处理的沉积物上的吸附行为亦可以用Freundlich等温线描述。
C.三种表面活性剂在H2O2处理的沉积物上的吸附等温线呈非线性,符合Freundlich型吸附等温线。吸附机理主要是沉积物中粘土矿物的表面吸附作用。
D.由于“盐析”作用的结果,导致表面活性剂在水体中的溶解度的降低和沉积物中可溶有机组分向溶液释放的减少,最终导致沉积物分配系数Kd随盐度增加而增加,表面活性剂的吸附能力增加。
E.酸度对三种表面活性剂吸附的影响因吸附质类型的不同而不同。Tween20在溶液中不离解,其吸附行为受pH影响不大;pH降低,沉积物表面负电性变得更弱,阴离子表面活性剂SDBS的烷基链与沉积物表面间的静电作用增强,使SDBS吸附能力增加。而对阳离子表面活性剂CTAB而言,此作用正好相反。
F.温度对三种表面活性剂吸附的影响较大,温度升高,有机物溶解度增加,疏水作用减弱;沉积物中可溶有机组分一部分向溶液中溶出,沉积物有机碳的分配作用会降低,结果使表面活性剂的吸附能力下降。
G.对表面活性剂在海洋沉积物上的吸附热力学函数的计算可知,ΔGθ< 0说明吸附过程是自发的;ΔHθ< 0证明了吸附过程是放热的;ΔSθ< 0说明吸附过程伴随着熵的减少。
总之,表面活性剂在海洋沉积物上的吸附过程是非常复杂的,不仅受沉积物组成的影响,一些外部因素如盐度、pH值、温度等的影响也很重要。
Surfactants are toxic organic pollutants, which are ubiquitous in the environment. They are also the basic raw materials of organic chemical industries. Wastewater containing surfactants has been let out to the marine environment, which has done great harm to the human being and marine organisms. Chemists and environmental researchers have paid much attention to it. Investigation on sorption behavior of surfactants on marine sediments is realistically significant to deeply study their transference and marine ecological effect. It can also provide the theoretical foundation for the pollution control.
The study objects of the dissertation referred to three surfactants, which are ubiquitous in marine environment and have carcinogenic harmful properties. There are lots of environmental, biological and geochemical significance on the research of the sorption behavior on marine sediments. Meanwhile, the research results of the thesis will definitely provide an effective and valuable evidence for marine scientific research and marine environment protection.
In this work, the sorption behavior of three kinds of typical surfactants, polyoxyethylene (20) sorbitan Monolaurate (Tween20), sodium dodecylbenzene sulfonate (SDBS) and cetyl trimethyl ammonium bromide (CTAB), in the system of marine sediment-seawater were comprehensively and deeply studied. A stress was made on the difference of sorption isotherms of the three surfactants on marine sediments treated by different means and the effect of salinity, acidity, temperature of seawater on their sorption behavior. The concrete results are shown as follows:
A. The sorption behavior of surfactants on marine sediments reached equilibrium within 50min, 100min, 1h for Tween20, SDBS, CTAB, respectively no matter what media (Natural Seawater-NSW, Diluted Seawater-DSW and Distilled Water-DW) were utilized. The sorption percentage varied with the media in the sequence of NSW>DSW>DW.
B. The sorption behavior of three kinds of surfactants on HCl- and H2O- treated sediments accorded well with the linear isotherm and the partition effect of sediment organic carbon played an important role during the process. At the same time, the behavior for SDBS also accorded with the Freundlich isotherm.
C. The sorption isotherms of three kinds of surfactants on H2O2-treated sediments presented nonlinear and could be depicted by the Freundlich model. The surface function and microporous adsorption of the clay significantly influenced the adsorption process.
D. The“salting out”effect of seawater led to the decrease in the solubilities of surfactants and the release of the solvable part of sediment organic carbon into aqueous solution. Accordingly, the partitioning coefficients Kd and sorption capacity of surfactants increased with the increase of salinity of seawater.
E. The effect of acidity on sorption of surfactants on sediments depended on their types. The effect was slight on Tween20 because it was undissociated in aqueous solutions. The decrease of pH might influence the surface charge of the sediments which became less negative with a consequent increase in electrostatic effect between alkyl chain of SDBS and the sediment surface. As a result, the capacity of adsorption of SDBS increased. The influence on CTAB was just opposite.
F. The effect of temperature on the adsorption of surfactants is obvious. The solubilities of surfactants would increase with increasing temperature; The affinity between surfactants and water molecules was strengthened; The organic matters in sediments were partially dissolved out into solution with increasing temperature and consequently the partition effect of sediment organic carbon decreased. Therefore, the capacity of sorption of sediments decreased.
G. The thermodynamic functions of Gibbs free energy(ΔGθ<0),enthalpy (ΔHθ<0) and entropy(ΔSθ<0) terms were determined, indicating that the sorption was a spontaneous and exothermic process which accompanied with a decrease in the degree of freedom.
In short, the adsorption process of surfactants on marine sediments is complex. It is influenced by not only the composition of sediments but also some external factors such as salinity, pH, temperature and so on.
本论文通过实验室模拟,研究了三种典型表面活性剂失水山梨醇聚氧乙烯(20)醚月桂酸酯(Tween20)、十二烷基苯磺酸钠(SDBS)、十六烷基三甲基溴化铵(CTAB)在海洋沉积物上的吸附行为,重点探讨了其在不同处理方式的海洋沉积物上的吸附等温线的差异及海水盐度、酸度、温度等环境因素对其吸附的影响。得到了如下结论:
A.无论在何种介质(天然海水NSW、稀释海水DSW、蒸馏水DW)中,Tween20在海洋沉积物上吸附达到平衡的时间约为50min,SDBS为100min,CTAB约为1h。吸附介质对平衡时间没有影响,但会影响沉积物对表面活性剂的吸附百分数,顺序如下:NSW>DSW>DW。
B.三种表面活性剂在HCl和水处理的沉积物上的吸附行为均可用线性吸附等温线描述,吸附主要是通过沉积物中有机碳的分配作用来完成的。SDBS在HCl和水处理的沉积物上的吸附行为亦可以用Freundlich等温线描述。
C.三种表面活性剂在H2O2处理的沉积物上的吸附等温线呈非线性,符合Freundlich型吸附等温线。吸附机理主要是沉积物中粘土矿物的表面吸附作用。
D.由于“盐析”作用的结果,导致表面活性剂在水体中的溶解度的降低和沉积物中可溶有机组分向溶液释放的减少,最终导致沉积物分配系数Kd随盐度增加而增加,表面活性剂的吸附能力增加。
E.酸度对三种表面活性剂吸附的影响因吸附质类型的不同而不同。Tween20在溶液中不离解,其吸附行为受pH影响不大;pH降低,沉积物表面负电性变得更弱,阴离子表面活性剂SDBS的烷基链与沉积物表面间的静电作用增强,使SDBS吸附能力增加。而对阳离子表面活性剂CTAB而言,此作用正好相反。
F.温度对三种表面活性剂吸附的影响较大,温度升高,有机物溶解度增加,疏水作用减弱;沉积物中可溶有机组分一部分向溶液中溶出,沉积物有机碳的分配作用会降低,结果使表面活性剂的吸附能力下降。
G.对表面活性剂在海洋沉积物上的吸附热力学函数的计算可知,ΔGθ< 0说明吸附过程是自发的;ΔHθ< 0证明了吸附过程是放热的;ΔSθ< 0说明吸附过程伴随着熵的减少。
总之,表面活性剂在海洋沉积物上的吸附过程是非常复杂的,不仅受沉积物组成的影响,一些外部因素如盐度、pH值、温度等的影响也很重要。
Surfactants are toxic organic pollutants, which are ubiquitous in the environment. They are also the basic raw materials of organic chemical industries. Wastewater containing surfactants has been let out to the marine environment, which has done great harm to the human being and marine organisms. Chemists and environmental researchers have paid much attention to it. Investigation on sorption behavior of surfactants on marine sediments is realistically significant to deeply study their transference and marine ecological effect. It can also provide the theoretical foundation for the pollution control.
The study objects of the dissertation referred to three surfactants, which are ubiquitous in marine environment and have carcinogenic harmful properties. There are lots of environmental, biological and geochemical significance on the research of the sorption behavior on marine sediments. Meanwhile, the research results of the thesis will definitely provide an effective and valuable evidence for marine scientific research and marine environment protection.
In this work, the sorption behavior of three kinds of typical surfactants, polyoxyethylene (20) sorbitan Monolaurate (Tween20), sodium dodecylbenzene sulfonate (SDBS) and cetyl trimethyl ammonium bromide (CTAB), in the system of marine sediment-seawater were comprehensively and deeply studied. A stress was made on the difference of sorption isotherms of the three surfactants on marine sediments treated by different means and the effect of salinity, acidity, temperature of seawater on their sorption behavior. The concrete results are shown as follows:
A. The sorption behavior of surfactants on marine sediments reached equilibrium within 50min, 100min, 1h for Tween20, SDBS, CTAB, respectively no matter what media (Natural Seawater-NSW, Diluted Seawater-DSW and Distilled Water-DW) were utilized. The sorption percentage varied with the media in the sequence of NSW>DSW>DW.
B. The sorption behavior of three kinds of surfactants on HCl- and H2O- treated sediments accorded well with the linear isotherm and the partition effect of sediment organic carbon played an important role during the process. At the same time, the behavior for SDBS also accorded with the Freundlich isotherm.
C. The sorption isotherms of three kinds of surfactants on H2O2-treated sediments presented nonlinear and could be depicted by the Freundlich model. The surface function and microporous adsorption of the clay significantly influenced the adsorption process.
D. The“salting out”effect of seawater led to the decrease in the solubilities of surfactants and the release of the solvable part of sediment organic carbon into aqueous solution. Accordingly, the partitioning coefficients Kd and sorption capacity of surfactants increased with the increase of salinity of seawater.
E. The effect of acidity on sorption of surfactants on sediments depended on their types. The effect was slight on Tween20 because it was undissociated in aqueous solutions. The decrease of pH might influence the surface charge of the sediments which became less negative with a consequent increase in electrostatic effect between alkyl chain of SDBS and the sediment surface. As a result, the capacity of adsorption of SDBS increased. The influence on CTAB was just opposite.
F. The effect of temperature on the adsorption of surfactants is obvious. The solubilities of surfactants would increase with increasing temperature; The affinity between surfactants and water molecules was strengthened; The organic matters in sediments were partially dissolved out into solution with increasing temperature and consequently the partition effect of sediment organic carbon decreased. Therefore, the capacity of sorption of sediments decreased.
G. The thermodynamic functions of Gibbs free energy(ΔGθ<0),enthalpy (ΔHθ<0) and entropy(ΔSθ<0) terms were determined, indicating that the sorption was a spontaneous and exothermic process which accompanied with a decrease in the degree of freedom.
In short, the adsorption process of surfactants on marine sediments is complex. It is influenced by not only the composition of sediments but also some external factors such as salinity, pH, temperature and so on.
引文
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