气态微量单质汞改性蛭石吸附剂及吸附机理的研究
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摘要
汞是一种剧毒性、高挥发性、在生物体内和食物链中具有永久累积性的有毒物质,在环保领域越来越受到重视。煤的燃烧是大气汞污染的一个主要来源。本文在介绍国内外气态单质汞治理技术的基础上,提出了利用廉价的蛭石吸附剂对气态单质汞控制的新思路。通过对蛭石吸附剂的研制,主要讨论了经不同浓度的盐酸以及三氯化铁浸渍蛭石对吸附的影响。最后优选出盐酸改性和三氯化铁改性蛭石。并对这两种蛭石进行了固定床吸附脱除微量气态单质汞的实验研究。实验结果表明:改性蛭石对气态单质汞的吸附与汞的进气浓度,吸附反应温度,吸附剂颗粒大小等因素均有关。其中汞进气浓度越高蛭石吸附的汞的量也就越多,但是此时总的汞的脱除率却是下降的;提高吸附反应温度或者在一定的程度内减小吸附剂颗粒的大小均可以提高汞的吸附容量,但是吸附剂的颗粒不易太小。最后又对改性蛭石和活性炭对单质汞吸附进行了对比,结果发现改性蛭石在较高温度下对单质汞的去除率已经优于活性炭,并且燃煤尾气的温度即使在经过了多个热交换器之后还是较高,因此可以预测改性蛭石吸附剂在实际烟气除汞当中具有实际的应用价值。
文章还对蛭石原土及盐酸改性后的蛭石进行了X射线衍射分析,结果显示改性后的蛭石与蛭石原土的XRD图谱的特征发生了明显的变化,一是谱形,二是衍射线的强度。改性蛭石样和蛭石原样相比,改性蛭石样中晶片间的距离d相对增大,并且部分谱峰消失,原因是酸溶蚀、分解了蛭石孔隙中的有机或无机杂质,疏通了孔道,使蛭石的晶片间距增大。表征结果证实了改性之后的蛭石吸附剂的吸附效果变好。
通过基本数学模型,建立了动力学方程式,并且对实验数据进行拟合,得出不同反应温度下吸附平衡常数、理论最大吸附量、不同温度下的吸附热以及吸附速度方程。具体数值为:25℃时,q_(max)=7.65~*10~(-6)g/g,k=4.0664~*10~4m~3/g,△H=3.54KJ/mol;70℃时,q_(max)=1.3034~*10~(-5)g/g,k=2.5596~*10~4m~3/g,△H=5.44 KJ/mol;140℃时,q_(max)=1.7883~*10~(-5)g/g,k=2.1620~*10~4m~3/g,△H=7.11KJ/mol。且25℃时盐酸改性蛭石4~#对单质汞的吸附速度方程为:q=q_e[1—exp(—22.9267t~(1.0638))]。
The mercury is a kind of violently poisonous,highly volatile substance and permanent accumulation virulent material in organism and the food chain.It has been more attention in the environmental protection domain.Coal combustion is a major source of atmospheric mercury pollution.After investigated some domestic and foreign technologies of removing Hg~0,a new method of removal gas-phase elementary mercury was put forward,such as cheap vermiculite adsorbents.Through the vermiculite adsorbents manufacture,mainly discussed the different concentrations of hydrochloric acid and ferric chloride impregnating vermiculite on the adsorption effects.Finally elect optimal vermiculite modified by HCl or FeCl_3.The experimental study of fixed-bed of two vermiculites adsorbing vapour-gas Hg~0 from flue gases has been investigated in this paper.The experimental results show that: Modified vermiculite adsorbed the gaseous state Hg~0.The adsorption effects are related to the entrance mercury concentration,adsorption reaction temperature and the difference of absorbent pellet size.The adsorption amounts could be improved when increasing the entrance mercury,but the removal efficiency of Hg~0 is to come down.The adsorption efficiency could be improved when improving the temperature of the adsorption or reducing diameter of the sorbents.But the adsorbents sizes are not suited of more little.At last modified vermiculite put up to contrast with active carbon.Results show that the removal effect of modified vermiculite is better than active carbon at relative high temperature.And the the temperature of combustion of flue-gas is more high after passing through several heat exchangers.So modified vermiculite can be forecasted that they are very valuable at the actual application.
Vermiculite and HCl modified vermiculite were determined by X-ray powder diffraction(XRD).The results show that the structure spectroscopy of HCl modified vermiculite was changed obviously.The fist is the structure spectroscopy,the second is the diffraction intensity;The space of interbedded crystal(d)about the modified vermiculite was increased relatively,and some structure spectroscopy are disappear,which is because the acid dissolving the organic and abio-organic impurity,dredging the hole,making the wafer space between vermiculite accretion.The result approved that the adsorption effect was getting better after the vermiculite modified.
Introduced some of the basic mathematical models,established kinetic equations,and carried on the fitting to the experiment data,obtained the adsorption equilibrium constant, the theory biggest adsorptive capacity,the heat of adsorption and the adsorption speed equation under the different reaction temperature.The concrete data indict that the temperature 25℃,q_(max)= 7.65~* 10~(-6)g/g,k=4.0664~* 10~4 m~3/g,△H=3.54KJ/mol;At the temperature 70℃,k = 2.5596~* 10~4 m~3/g,q_(max)=1.3034~* 10~5 g/g,△H=5.44 KJ/mol;At the temperature 140℃,k=2.1620~* 10~4 m~3/g,q_(max)= 1.7883~* 10~(-5)g/g,△H=7.11 KJ/mol.And the modified vermiculite 4~# of hydrochloric acid to Hg~0 adsorption speed equation shows as follow:q = q_e[1 - exp(-22.9267t~(1.0638))]。
文章还对蛭石原土及盐酸改性后的蛭石进行了X射线衍射分析,结果显示改性后的蛭石与蛭石原土的XRD图谱的特征发生了明显的变化,一是谱形,二是衍射线的强度。改性蛭石样和蛭石原样相比,改性蛭石样中晶片间的距离d相对增大,并且部分谱峰消失,原因是酸溶蚀、分解了蛭石孔隙中的有机或无机杂质,疏通了孔道,使蛭石的晶片间距增大。表征结果证实了改性之后的蛭石吸附剂的吸附效果变好。
通过基本数学模型,建立了动力学方程式,并且对实验数据进行拟合,得出不同反应温度下吸附平衡常数、理论最大吸附量、不同温度下的吸附热以及吸附速度方程。具体数值为:25℃时,q_(max)=7.65~*10~(-6)g/g,k=4.0664~*10~4m~3/g,△H=3.54KJ/mol;70℃时,q_(max)=1.3034~*10~(-5)g/g,k=2.5596~*10~4m~3/g,△H=5.44 KJ/mol;140℃时,q_(max)=1.7883~*10~(-5)g/g,k=2.1620~*10~4m~3/g,△H=7.11KJ/mol。且25℃时盐酸改性蛭石4~#对单质汞的吸附速度方程为:q=q_e[1—exp(—22.9267t~(1.0638))]。
The mercury is a kind of violently poisonous,highly volatile substance and permanent accumulation virulent material in organism and the food chain.It has been more attention in the environmental protection domain.Coal combustion is a major source of atmospheric mercury pollution.After investigated some domestic and foreign technologies of removing Hg~0,a new method of removal gas-phase elementary mercury was put forward,such as cheap vermiculite adsorbents.Through the vermiculite adsorbents manufacture,mainly discussed the different concentrations of hydrochloric acid and ferric chloride impregnating vermiculite on the adsorption effects.Finally elect optimal vermiculite modified by HCl or FeCl_3.The experimental study of fixed-bed of two vermiculites adsorbing vapour-gas Hg~0 from flue gases has been investigated in this paper.The experimental results show that: Modified vermiculite adsorbed the gaseous state Hg~0.The adsorption effects are related to the entrance mercury concentration,adsorption reaction temperature and the difference of absorbent pellet size.The adsorption amounts could be improved when increasing the entrance mercury,but the removal efficiency of Hg~0 is to come down.The adsorption efficiency could be improved when improving the temperature of the adsorption or reducing diameter of the sorbents.But the adsorbents sizes are not suited of more little.At last modified vermiculite put up to contrast with active carbon.Results show that the removal effect of modified vermiculite is better than active carbon at relative high temperature.And the the temperature of combustion of flue-gas is more high after passing through several heat exchangers.So modified vermiculite can be forecasted that they are very valuable at the actual application.
Vermiculite and HCl modified vermiculite were determined by X-ray powder diffraction(XRD).The results show that the structure spectroscopy of HCl modified vermiculite was changed obviously.The fist is the structure spectroscopy,the second is the diffraction intensity;The space of interbedded crystal(d)about the modified vermiculite was increased relatively,and some structure spectroscopy are disappear,which is because the acid dissolving the organic and abio-organic impurity,dredging the hole,making the wafer space between vermiculite accretion.The result approved that the adsorption effect was getting better after the vermiculite modified.
Introduced some of the basic mathematical models,established kinetic equations,and carried on the fitting to the experiment data,obtained the adsorption equilibrium constant, the theory biggest adsorptive capacity,the heat of adsorption and the adsorption speed equation under the different reaction temperature.The concrete data indict that the temperature 25℃,q_(max)= 7.65~* 10~(-6)g/g,k=4.0664~* 10~4 m~3/g,△H=3.54KJ/mol;At the temperature 70℃,k = 2.5596~* 10~4 m~3/g,q_(max)=1.3034~* 10~5 g/g,△H=5.44 KJ/mol;At the temperature 140℃,k=2.1620~* 10~4 m~3/g,q_(max)= 1.7883~* 10~(-5)g/g,△H=7.11 KJ/mol.And the modified vermiculite 4~# of hydrochloric acid to Hg~0 adsorption speed equation shows as follow:q = q_e[1 - exp(-22.9267t~(1.0638))]。
引文
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