粘土材料及膨胀石墨对海水中柴油的吸附及其机理研究
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摘要
在处理海上溢油时,吸油材料因能起到集中和临时固定油的作用而得到广泛应用。环保型吸附材料具有吸附量大、价格低、使用方便、后处理不会产生二次污染的特点,既可以将溢油回收,又可避免带来新的环境问题,具有广阔的应用前景。因此,寻求环境友好型的吸附材料,开展其在海水除油中的应用研究具有重要的现实意义。
本论文选用几种粘土材料(有机改性膨润土、硅藻土、钠基膨润土)和膨胀石墨,研究了其对海水中柴油污染物的吸附性能。在吸附动力学研究的基础上,开展了吸附等温线的研究,并探讨了吸附机理。论文通过正交试验研究了多种因素对除油效果的影响,并对吸附条件进行了优化。通过比较几种吸附材料的平衡吸附量、价格及后续处理的难易程度,提出了合理的实施方案。本实验采用紫外分光光度法测定海水中的含油量,通过试验得出了以下主要结论:
1、通过吸附动力学试验,建立有机改性膨润土、膨胀石墨、硅藻土和钠基膨润土对油吸附的二级动力学方程,得到平衡吸附量分别为3271、3078,1525和1212mg/g,平衡时间分别是15.18、18.92、36.15和48.39min。
2、吸油材料对海水中油的去除率随着投加量的增加而增加,随着海水含油量的增加而减小;在实验研究范围内,有机改性膨润土、膨胀石墨、硅藻土和钠基膨润土对海水中油的去除率都随着温度、盐度和振荡频率的增加而增加。
3、随着油污染海水pH值的增大,膨胀石墨、硅藻土和钠基膨润土对海水中浮油的去除率都有减小的趋势;而有机改性膨润土在pH值为8的条件下,除油效果较好。
4、有机改性膨润土和硅藻土对海水中油的吸附等温线符合Freundlich吸附等温方程;膨胀石墨和钠基膨润土对海水中油的吸附过程,可用Langmuir吸附等温式和Freundlich吸附等温式来描述,其中Langmuir吸附等温式更为贴切。
5、有机改性膨润土对海水中柴油的吸附主要通过层间有机相的分配作用而实现;膨胀石墨的吸油机理是表面吸附和填充空间吸油;硅藻土的吸附机理主要有微孔吸附和表面配位吸附;钠基膨润土的吸油机理包括表面吸附和分配作用。热力学计算证明四种吸油材料对海水中柴油的吸附均属于物理吸附。
6、影响有机改性膨润土、膨胀石墨、硅藻土和钠基膨润土的对海水中油的吸附的主次因素分别为:盐度＞pH＞振荡频率＞温度;温度＞振荡频率＞盐度＞pH;pH＞盐度＞温度＞振荡频率;pH＞盐度＞温度＞振荡频率。
7、综合吸油材料的除油效果、技术经济比较及后续处理的难易程度,认为四种吸油材料中,有机膨润土最具有实际应用的优势和潜力,较适合用于海洋溢油处理。
In dealing with oil spills at sea,the oil-absorbing material was widely used because they can concentrate and retain oil.Environmental friendly oil-absorbing materials have larger adsorption capacity and low price,and they can be easily used and would not produce secondary pollution.Environmental friendly oil-absorbing materials can make oil recycled and avoid new environmental problems,and they have broad application prospects.Therefore,the search for environment-friendly oil-absorbing materials.and carry out the applied research has a great practical significance.
In this paper,we selected clay material(modified organobentonite,diatomaceous earth,Na-bentonite) and exfoliate graphite and studied Adsorption of pollutants on the performance of diesel.The adsorption kinetics,adsorption isotherm were studied and to explore the adsorption mechanism.By orthogonal on the adsorption conditions were optimized.By comparing the number of adsorption equilibrium adsorption capacity, price and ease of follow-up,made a reasonable implementation.This experiment using UV spectrophotometric determination of oil content of seawater through the test produced the following major conclusions:
1.Through the adsorption kinetics experiment,secondary absorption kinetic equation of modified organobentonite,exfoliate graphite,diatomaceous earth and Na-bentonite are established.The equilibrium adsorption capacity of modified organobentonite,exfoliate graphite,diatomaceous earth and Na-bentonite is 3271,3078,1525 and 1212 mg/g respectively,and equilibrium time is 15.18,18.92 36.15 and 48.39 min respectively.
2.Oil removal efficiency increased with the increase of adsorbing material added in the system,and decreased with the increase of original oil content in seawater,in the scope of the study in the experiment,the modified organobentonite,exfoliate graphite,diatomaceous earth and Na-bentonite in seawater with the oil removal rate are increased with temperature,salinity and oscillation frequency.
3.With the oil pollution of seawater pH values increase,exfoliate graphite,diatomaceous earth and Na-bentonite in the oil removal rate has decreased;and the modified organobentonite in the pH value of 8,the removal can be achieved better results.
4.The adsorption isotherms of modified organobentonite and diatomaceous earth can be described as Freundlich's equation.The adsorption isotherms of exfoliate graphite and Na-bentonite can be used Langmuir isotherm and Freundlich isotherm to describe,The Langmuir isotherm is more appropriate.
5.Modified organobentonite absorption of oil,primarily through inter-layer organic phase,which plays a role in distribution;The absorption mechanism of exfoiiate graphite are surface absorption and oil-filled space absorption,of which spaces fill accounted for one of the main part;The adsorption mechanism of diatomaceous earth are mainly microporous coordination absorption and surface adsorption:Na-bentonite including the absorption mechanism of the surface absorption and the role of organic matter distribution.Thermodynamic calculations of modified organobentonite,exfoliate graphite,diatomaceous earth and Na-bentonite on the adsorption of diesel oil is physical adsorption.
6.The impact of modified organobentonite for oil adsorption followed by the main factors:salinity＞pH＞oscillation frequency＞temperature.The impact of exfoliate gaphite for oil adsorption followed by the main factors:temperature＞oscillation frequency＞salinity＞pH.The impact of diatomaceous earth for oil adsorption followed by the main factors:pH＞salinity＞temperature＞oscillation frequency.The impact of Na-bentonite for oil adsorption followed by the main factors: pH＞salinity＞temperature＞oscillation frequency.
7.Comparison of the effect of oil-absorbing materials,oil,technology economy and ease of follow-up treatment.Consider the four types of oil-absorbing materials.modidied organobentonite has most advantages and potential in practical application..it is more suitable for the treatment of sea spills.
本论文选用几种粘土材料(有机改性膨润土、硅藻土、钠基膨润土)和膨胀石墨,研究了其对海水中柴油污染物的吸附性能。在吸附动力学研究的基础上,开展了吸附等温线的研究,并探讨了吸附机理。论文通过正交试验研究了多种因素对除油效果的影响,并对吸附条件进行了优化。通过比较几种吸附材料的平衡吸附量、价格及后续处理的难易程度,提出了合理的实施方案。本实验采用紫外分光光度法测定海水中的含油量,通过试验得出了以下主要结论:
1、通过吸附动力学试验,建立有机改性膨润土、膨胀石墨、硅藻土和钠基膨润土对油吸附的二级动力学方程,得到平衡吸附量分别为3271、3078,1525和1212mg/g,平衡时间分别是15.18、18.92、36.15和48.39min。
2、吸油材料对海水中油的去除率随着投加量的增加而增加,随着海水含油量的增加而减小;在实验研究范围内,有机改性膨润土、膨胀石墨、硅藻土和钠基膨润土对海水中油的去除率都随着温度、盐度和振荡频率的增加而增加。
3、随着油污染海水pH值的增大,膨胀石墨、硅藻土和钠基膨润土对海水中浮油的去除率都有减小的趋势;而有机改性膨润土在pH值为8的条件下,除油效果较好。
4、有机改性膨润土和硅藻土对海水中油的吸附等温线符合Freundlich吸附等温方程;膨胀石墨和钠基膨润土对海水中油的吸附过程,可用Langmuir吸附等温式和Freundlich吸附等温式来描述,其中Langmuir吸附等温式更为贴切。
5、有机改性膨润土对海水中柴油的吸附主要通过层间有机相的分配作用而实现;膨胀石墨的吸油机理是表面吸附和填充空间吸油;硅藻土的吸附机理主要有微孔吸附和表面配位吸附;钠基膨润土的吸油机理包括表面吸附和分配作用。热力学计算证明四种吸油材料对海水中柴油的吸附均属于物理吸附。
6、影响有机改性膨润土、膨胀石墨、硅藻土和钠基膨润土的对海水中油的吸附的主次因素分别为:盐度＞pH＞振荡频率＞温度;温度＞振荡频率＞盐度＞pH;pH＞盐度＞温度＞振荡频率;pH＞盐度＞温度＞振荡频率。
7、综合吸油材料的除油效果、技术经济比较及后续处理的难易程度,认为四种吸油材料中,有机膨润土最具有实际应用的优势和潜力,较适合用于海洋溢油处理。
In dealing with oil spills at sea,the oil-absorbing material was widely used because they can concentrate and retain oil.Environmental friendly oil-absorbing materials have larger adsorption capacity and low price,and they can be easily used and would not produce secondary pollution.Environmental friendly oil-absorbing materials can make oil recycled and avoid new environmental problems,and they have broad application prospects.Therefore,the search for environment-friendly oil-absorbing materials.and carry out the applied research has a great practical significance.
In this paper,we selected clay material(modified organobentonite,diatomaceous earth,Na-bentonite) and exfoliate graphite and studied Adsorption of pollutants on the performance of diesel.The adsorption kinetics,adsorption isotherm were studied and to explore the adsorption mechanism.By orthogonal on the adsorption conditions were optimized.By comparing the number of adsorption equilibrium adsorption capacity, price and ease of follow-up,made a reasonable implementation.This experiment using UV spectrophotometric determination of oil content of seawater through the test produced the following major conclusions:
1.Through the adsorption kinetics experiment,secondary absorption kinetic equation of modified organobentonite,exfoliate graphite,diatomaceous earth and Na-bentonite are established.The equilibrium adsorption capacity of modified organobentonite,exfoliate graphite,diatomaceous earth and Na-bentonite is 3271,3078,1525 and 1212 mg/g respectively,and equilibrium time is 15.18,18.92 36.15 and 48.39 min respectively.
2.Oil removal efficiency increased with the increase of adsorbing material added in the system,and decreased with the increase of original oil content in seawater,in the scope of the study in the experiment,the modified organobentonite,exfoliate graphite,diatomaceous earth and Na-bentonite in seawater with the oil removal rate are increased with temperature,salinity and oscillation frequency.
3.With the oil pollution of seawater pH values increase,exfoliate graphite,diatomaceous earth and Na-bentonite in the oil removal rate has decreased;and the modified organobentonite in the pH value of 8,the removal can be achieved better results.
4.The adsorption isotherms of modified organobentonite and diatomaceous earth can be described as Freundlich's equation.The adsorption isotherms of exfoliate graphite and Na-bentonite can be used Langmuir isotherm and Freundlich isotherm to describe,The Langmuir isotherm is more appropriate.
5.Modified organobentonite absorption of oil,primarily through inter-layer organic phase,which plays a role in distribution;The absorption mechanism of exfoiiate graphite are surface absorption and oil-filled space absorption,of which spaces fill accounted for one of the main part;The adsorption mechanism of diatomaceous earth are mainly microporous coordination absorption and surface adsorption:Na-bentonite including the absorption mechanism of the surface absorption and the role of organic matter distribution.Thermodynamic calculations of modified organobentonite,exfoliate graphite,diatomaceous earth and Na-bentonite on the adsorption of diesel oil is physical adsorption.
6.The impact of modified organobentonite for oil adsorption followed by the main factors:salinity＞pH＞oscillation frequency＞temperature.The impact of exfoliate gaphite for oil adsorption followed by the main factors:temperature＞oscillation frequency＞salinity＞pH.The impact of diatomaceous earth for oil adsorption followed by the main factors:pH＞salinity＞temperature＞oscillation frequency.The impact of Na-bentonite for oil adsorption followed by the main factors: pH＞salinity＞temperature＞oscillation frequency.
7.Comparison of the effect of oil-absorbing materials,oil,technology economy and ease of follow-up treatment.Consider the four types of oil-absorbing materials.modidied organobentonite has most advantages and potential in practical application..it is more suitable for the treatment of sea spills.
引文
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