阳离子表面活性剂和重油复合体系在海洋沉积物上的吸附行为
摘要
复合污染已经成为环境化学发展的重要方向之一。随着工农业的发展,越来越多的有机污染物进入环境中,使得绝对意义上的单一环境污染不再存在。共存污染物之间存在的复杂交互作用,使得复合污染的环境行为及其影响已经变得越来越明显。一种有机污染物在环境中的吸附行为不仅受制于有机污染物自身的理化性质,沉积物(土壤)的化学组成、结构,而且常常受到环境因素(温度、盐度、共存有机污染物等)的影响。
石油类污染物和表面活性剂是海洋中常见的有机污染物,已经对人类和海洋生物造成极大影响,引起了化学家和环境学家的广泛重视。海洋沉积物对石油类污染物和表面活性剂的吸附是影响它们在环境中行为和归宿的主要因素之一,研究石油类污染物和表面活性剂共存时二者在海洋沉积物上的吸附行为,有利于了解它们在环境中的迁移转化,对我国的海洋科学和环境科学研究都具有很好的现实意义。
本论文以人工海水为介质,重点以重油和阳离子表面活性剂十六烷基三甲基溴化铵(CTAB)为研究对象,探讨了复合污染中其在胶州湾沉积物上的吸附动力学和吸附热力学行为,研究了介质(盐度)、温度等因素对重油和CTAB在沉积物上吸附行为的影响。主要得到以下结论：
(1)动力学研究表明重油-CTAB复合体系中沉积物对重油和CTAB的吸附动力学过程可以用伪二级动力学模型进行较好的描述。
(2)重油-CTAB复合体系中重油和CTAB在沉积物上的吸附等温线均为非线性,均较好的符合Freundlich等温式。(3)重油-CTAB复合体系中,沉积物对重油的吸附量随着CTAB初始浓度的增加,盐度的增加,温度的降低而增加；沉积物对CTAB的吸附量随着重油初始浓度的减小,盐度的增加,温度的降低而增加。
(4)热力学研究表明沉积物对重油的吸附热力学函数为ΔG0<0,ΔH0<0,ΔS0<0,表明重油在海洋沉积物上的吸附为物理吸附,是一个自发、放热、熵减小的过程。而沉积物对CTAB的吸附热力学函数为ΔG0<0,ΔH0<0,ΔS0>0,表明CTAB在海洋沉积物上的吸附该吸附是一个白发、放热、熵增加的过程。
Combined pollution has become one of the important directions of environmental chemistry at present. With the development of agriculture and industry, there have been more and more organic contaminants in combined polluted environment and interaction between two coexistent organic compounds has become increasingly apparent.The sorption of an organic contaminants on sediments(soils) depends on the physico-chemical properties of the chemical,the sediment characteristics (composition, surface area,pore size, and surface functional groups).Some studies show the effects of the environmental factors (temperature, salinity, coexistent organic compounds,etc).
Oil and surfactants are toxic organic pollutants,which are ubiquitous in the marine environment.They have done great harm to the human being and marine organisms.Chemists and environmental researchers have paid much attention to them. The sorption of is a main factor in controlling the fate and transport of oil and surfactants in the environment,and investigation on sorption behaviors of oil /surfactants on marine sendiments in combined polluted environment is very important from the practical points of view of the oceanic and environmental science.
In this thesis the parameters of sorption kinetics and thermodynamics of heavy oil and cationic surfactants cetyltrimethylammonium bromide(CTAB) on JiaozhouBay sediment are studied in artificial seawater. Furthermore, the effects of other environmental factors such as salinity.temperature are also investigated in combined polluted environment. The probable sorption mechanisms were discussed on the basis of the investigated data. The main results are as follows:
(1)The results showed that the sorption kinetic process of heavy oil and CTAB on sediment can be described by the Pesudo-second-order kinetic rate equation in combined polluted environment.
(2) The sorption isotherms of heavy oil and CTAB on sediments presented nonlinear and were well described by the Freundlich equation in combined polluted environment.
(3) In combined polluted environment,the sorption of heavy oil was favorably influenced by increasing initial CTAB concentration,salinity and decreasing temperatures;the sorption capability of CTAB on sediment increased with decreasing initial heavy oil concentration and temperatures and increasing salinity.
(4) The thermodynamic parameters(ΔG0<0,ΔH0<0,ΔS0<0) for heavy oil on sediments were calculated.which, indicated that the sorptions were physical processes and were spontaneous and exothermic with a decrease randomness.The thermodynamic parameters(ΔG0<0,ΔH0<0,ΔS0>0) for CTAB on sediments in presence of heavy oil were also calculated,,which,indicated that the sorption was spontaneous and exothermic.the randomness at the solid-liquid interface was increased during the process.
石油类污染物和表面活性剂是海洋中常见的有机污染物,已经对人类和海洋生物造成极大影响,引起了化学家和环境学家的广泛重视。海洋沉积物对石油类污染物和表面活性剂的吸附是影响它们在环境中行为和归宿的主要因素之一,研究石油类污染物和表面活性剂共存时二者在海洋沉积物上的吸附行为,有利于了解它们在环境中的迁移转化,对我国的海洋科学和环境科学研究都具有很好的现实意义。
本论文以人工海水为介质,重点以重油和阳离子表面活性剂十六烷基三甲基溴化铵(CTAB)为研究对象,探讨了复合污染中其在胶州湾沉积物上的吸附动力学和吸附热力学行为,研究了介质(盐度)、温度等因素对重油和CTAB在沉积物上吸附行为的影响。主要得到以下结论：
(1)动力学研究表明重油-CTAB复合体系中沉积物对重油和CTAB的吸附动力学过程可以用伪二级动力学模型进行较好的描述。
(2)重油-CTAB复合体系中重油和CTAB在沉积物上的吸附等温线均为非线性,均较好的符合Freundlich等温式。(3)重油-CTAB复合体系中,沉积物对重油的吸附量随着CTAB初始浓度的增加,盐度的增加,温度的降低而增加；沉积物对CTAB的吸附量随着重油初始浓度的减小,盐度的增加,温度的降低而增加。
(4)热力学研究表明沉积物对重油的吸附热力学函数为ΔG0<0,ΔH0<0,ΔS0<0,表明重油在海洋沉积物上的吸附为物理吸附,是一个自发、放热、熵减小的过程。而沉积物对CTAB的吸附热力学函数为ΔG0<0,ΔH0<0,ΔS0>0,表明CTAB在海洋沉积物上的吸附该吸附是一个白发、放热、熵增加的过程。
Combined pollution has become one of the important directions of environmental chemistry at present. With the development of agriculture and industry, there have been more and more organic contaminants in combined polluted environment and interaction between two coexistent organic compounds has become increasingly apparent.The sorption of an organic contaminants on sediments(soils) depends on the physico-chemical properties of the chemical,the sediment characteristics (composition, surface area,pore size, and surface functional groups).Some studies show the effects of the environmental factors (temperature, salinity, coexistent organic compounds,etc).
Oil and surfactants are toxic organic pollutants,which are ubiquitous in the marine environment.They have done great harm to the human being and marine organisms.Chemists and environmental researchers have paid much attention to them. The sorption of is a main factor in controlling the fate and transport of oil and surfactants in the environment,and investigation on sorption behaviors of oil /surfactants on marine sendiments in combined polluted environment is very important from the practical points of view of the oceanic and environmental science.
In this thesis the parameters of sorption kinetics and thermodynamics of heavy oil and cationic surfactants cetyltrimethylammonium bromide(CTAB) on JiaozhouBay sediment are studied in artificial seawater. Furthermore, the effects of other environmental factors such as salinity.temperature are also investigated in combined polluted environment. The probable sorption mechanisms were discussed on the basis of the investigated data. The main results are as follows:
(1)The results showed that the sorption kinetic process of heavy oil and CTAB on sediment can be described by the Pesudo-second-order kinetic rate equation in combined polluted environment.
(2) The sorption isotherms of heavy oil and CTAB on sediments presented nonlinear and were well described by the Freundlich equation in combined polluted environment.
(3) In combined polluted environment,the sorption of heavy oil was favorably influenced by increasing initial CTAB concentration,salinity and decreasing temperatures;the sorption capability of CTAB on sediment increased with decreasing initial heavy oil concentration and temperatures and increasing salinity.
(4) The thermodynamic parameters(ΔG0<0,ΔH0<0,ΔS0<0) for heavy oil on sediments were calculated.which, indicated that the sorptions were physical processes and were spontaneous and exothermic with a decrease randomness.The thermodynamic parameters(ΔG0<0,ΔH0<0,ΔS0>0) for CTAB on sediments in presence of heavy oil were also calculated,,which,indicated that the sorption was spontaneous and exothermic.the randomness at the solid-liquid interface was increased during the process.
引文
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