活性炭在袋式除尘器内脱除元素汞的实验研究与数值模拟
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摘要
汞是煤中存在的微量元素之一,在煤燃烧过程中随着烟气排放到自然环境中。汞污染物具有生理毒性,能在生物体内以及食物链中累积,所以人们对汞污染控制的关注程度越来越高。我国目前的能源结构是以煤为主,由于燃煤所引发的汞污染已成为主要的环境问题之一,政府相关部门及研究学者正在积极开展汞污染控制的研究工作。依托国家高技术研究发展计划项目(863计划)“基于干法联合脱除难捕集燃煤可吸入颗粒物及重金属关键技术研究”(编号：2008AA05Z305),利用同时脱除燃煤烟气中可吸入颗粒物及元素汞的装置,对活性炭在除尘器中吸附脱除烟气中的元素汞展开研究。
分析了我国煤消费以及煤中汞含量的基本情况,阐述了煤在燃烧全过程中,汞形态的迁移及转化。结合活性炭喷射控制烟气汞排放技术,着重对汞在吸附反应器和袋式除尘器中去除的影响因素进行了实验研究,同时分析了除尘器中粉尘层对汞脱除的影响。结合实验研究,提出了袋式除尘器空间活性炭汞吸附模型。通过浸渍和烧结的方法制备了负载氧化锰的活性炭纤维,并利用先进的材料表征技术进行了表征,在固定床中研究了其对元素汞的吸附去除能力,初步分析了其脱除元素汞的机理。
利用并流吸附反应器,以活性炭为吸附剂,进行了脱汞实验研究。结果表明：活性炭对元素汞的脱除效率随着吸附反应温度的升高而降低,吸附反应温度越高,元素汞的脱除效率越低。当温度为80℃、120℃和150℃时,活性炭对元素汞的脱除率的分别为46.3%、44.0%和40.0%；汞脱除率随着碳汞比的增大而增大；当碳汞比为4000、6000和8000的条件下,并流吸附反应器脱汞效率分别达到31.3%、34.7%和40.0%。
以活性炭为吸附剂,在袋式除尘器中考察了对元素汞的吸附脱除特性。研究中把除尘器中活性炭对元素汞的脱除作用分成两部分,分别是除尘器空间和粉尘层,并着重研究分析了滤袋上粉尘层的存在对脱汞效率的影响。结果表明：随着碳汞比的增加,脱汞效率明显提高。当碳汞比为4000、6000和8000时,除尘器中汞的脱除效率分别为30.4%、34.6%和40.3%,粉尘层对汞的脱除效率分别为3.65%、3.20%、3.66%。在除尘器中元素汞的脱除,其中除尘器空间作出了主要贡献,粉尘层只起了很小一部分作用,并且碳汞比的变化对粉尘层吸附元素汞的影响很小。可以利用袋式除尘器作为活性炭的吸附反应场所,强化对元素汞的吸附去除,从而减少燃煤烟气中汞的排放。
在并流吸附反应器和袋式除尘器中,利用活性炭吸附元素汞研究的基础上,建立了袋式除尘器空间活性炭汞吸附模型。利用所建立的模型,讨论了元素汞初始浓度、气布比、温度、碳汞比和颗粒粒径对脱汞效率的影响。模型的建立对利用活性炭喷射技术,控制烟气汞排放的实验研究和工程工艺优化提供了建议。
利用浸渍烧结的方法,制备了负载氧化锰的活性炭纤维(activated carbon fiber, ACF),对负载后材料用TEM、XRD、XPS和FTIR进行了表征,结果表明氧化锰在ACF表面分散良好,颗粒粒径在50nm左右。ACF表面氧化锰的形式为MnO和MnO2。负载后的ACF表面C-OH、C=O、COOH的含量增加。利用负载后材料进行了吸附元素汞的实验,研究结果表明：负载后的ACF吸附汞的穿透时间大大延长。浸渍液浓度对氧化锰的负载量有明显影响,锰负载量为6.7at.%,对汞的去除效率最佳。在150℃时,负载氧化锰后的ACF对元素汞表现出良好的吸附性能。
研究表明活性炭在袋式除尘器中对元素汞的吸附为物理吸附,所建立的吸附模型可以预测操作参数对活性炭吸附元素汞的影响。制备的负载氧化锰的活性炭纤维新型过滤材料对元素汞的吸附为化学吸附,促进了对元素汞的吸附去除。本研究对利用袋式除尘器对烟气中元素汞的去除具有工程指导意义。
Mercury is one of the trace elements in the presence of coal, and it is emitted into the environment with the flue gas in the process of coal combustion. Because of its bioaccumulation and physiological toxicity, mercury pollution control is raised more attention. Mercury pollution caused by coal combustion, has been one of the major environmental problems in China, due to the coal-dominated energy structure. The research on mercury pollution controls technology has been actively carrying out by relevant government departments and scholars. This research is focused on elemental mercury removed by activated carbon in fabric filter, with the support of the National High Technology Research and Development Program (No:2008AA05Z305).
The situation of coal consumption and mercury content in our country was described, the migration and transformation of mercury in the whole process of coal combustion was also explained. The factors affecting on elemental mercury removal by activated carbon both in entrained-flow adsorption reactor and fabric filter were studied, the mercury removal efficiency of dust cake on filter surface was analyzed in detail. The model of mercury sorption by activated carbon in the chamber of filter was established. The load of manganese oxide on activated carbon fiber was prepared and characterized, and the removal capacity of elemental mercury was studied.
The elemental mercury removal capability in the entrained-flow adsorption reactor was investigated using activated carbon as adsorbent. The results showed that:the higher the adsorption temperature, the lower the elemental mercury removal efficiency. When the temperature were at 80℃、120℃、and 150℃, the elemental mercury removal efficiency of activated carbon were reached 46.3%、44.0% and 40.0% respectively。The mercury removal efficiency increases with the C/Hg ratio (mass ratio of injected carbon to mercury) increases, the mercury removal efficiency were 31.3%,34.7%、40.0%, under the C/Hg ratio at 4000,6000 and 8000 respectively
The elemental mercury removal capability in fabric filter was investigated using activated carbon as adsorbent. The total amount of Hg0 adsorption in the fabric filter can be divided into two parts, the amount of Hg0 adsorbed by the activated carbon collected on the filter surface, and the rest removed by the activated carbon somewhere inside the fabric filter. The elemental mercury removal efficiency of fabric filter in the presence of dust cake on the filter surface was investigated in detail. The results showed that:the elemental mercury removal efficiency was significantly improved with the C/Hg ratio increases. The mercury removal efficiency of the activated carbon inside the fabric filter was 30.4%、34.6%、40.3%, under the C/Hg ratio at 4000、6000 and 8000 respectively. But, the mercury removal efficiency of the activated carbon particles collected on the filter surface only reached 3.65%、3.20%、3.66% respectively, The chamber of filter made a major contribution to the mercury removal efficiency, and the dust cake is only a small part of the role. The change of C/Hg ratio has little effect on the elemental mercury removal of the dust cake. Fabric filter can be used as activated carbon adsorption reaction sites, for reducing mercury emissions from coal-fired flue gas.
Based on the results of elemental mercury removal by activated carbon in the entrained-flow reactor and fabric filter, the model of mercury sorption by activated carbon in the chamber of filter was established. The factors affecting the elemental mercury adsorption on activated carbon were discussed, such as:C/Hg ratio, particle diameter, flue-gas temperature, flue-gas velocity, mercury concentration, using the present adsorption model.
The manganese oxide was loaded on the activated carbon fiber (ACF) by impregnating and sintering. The samples of ACF were characterized before and after loading, using TEM、XPS、XRD and FTIR. The results show that manganese oxide was well dispersed on the surface of ACF. The particle diameter was about 50nm. The presence of manganese form was MnO and MnO2. The amount of C-OH、C=O、COOH was increased after loading on the surface of ACF. The adsorption ability of elemental mercury before and after modification was also studied. The breakthrough time was greatly extended after loading. The concentration of impregnating solution had a significant effect on the content of manganese on ACF. The removal efficiency of elemental mercury reached the best when the manganese content on the ACF surface was 6.7at.%. The loaded ACF showed a good adsorption property of elemental mercury at 150℃. The initial concentration of elemental mercury has an impact on the removal efficiency of elemental mercury.
It is shown that elemental mercury adsorption removal by activated carbon in the bag filter is physical adsorption. The adsorption model can predict the impact of operating parameters on the activated carbon adsorption of elemental mercury. The adsorption of elemental mercury by the loaded ACF is chemical adsorption. It can promote the adsorption removal of elemental mercury. This study has a practical significance in the removal of elemental mercury by fabric filter.
分析了我国煤消费以及煤中汞含量的基本情况,阐述了煤在燃烧全过程中,汞形态的迁移及转化。结合活性炭喷射控制烟气汞排放技术,着重对汞在吸附反应器和袋式除尘器中去除的影响因素进行了实验研究,同时分析了除尘器中粉尘层对汞脱除的影响。结合实验研究,提出了袋式除尘器空间活性炭汞吸附模型。通过浸渍和烧结的方法制备了负载氧化锰的活性炭纤维,并利用先进的材料表征技术进行了表征,在固定床中研究了其对元素汞的吸附去除能力,初步分析了其脱除元素汞的机理。
利用并流吸附反应器,以活性炭为吸附剂,进行了脱汞实验研究。结果表明：活性炭对元素汞的脱除效率随着吸附反应温度的升高而降低,吸附反应温度越高,元素汞的脱除效率越低。当温度为80℃、120℃和150℃时,活性炭对元素汞的脱除率的分别为46.3%、44.0%和40.0%；汞脱除率随着碳汞比的增大而增大；当碳汞比为4000、6000和8000的条件下,并流吸附反应器脱汞效率分别达到31.3%、34.7%和40.0%。
以活性炭为吸附剂,在袋式除尘器中考察了对元素汞的吸附脱除特性。研究中把除尘器中活性炭对元素汞的脱除作用分成两部分,分别是除尘器空间和粉尘层,并着重研究分析了滤袋上粉尘层的存在对脱汞效率的影响。结果表明：随着碳汞比的增加,脱汞效率明显提高。当碳汞比为4000、6000和8000时,除尘器中汞的脱除效率分别为30.4%、34.6%和40.3%,粉尘层对汞的脱除效率分别为3.65%、3.20%、3.66%。在除尘器中元素汞的脱除,其中除尘器空间作出了主要贡献,粉尘层只起了很小一部分作用,并且碳汞比的变化对粉尘层吸附元素汞的影响很小。可以利用袋式除尘器作为活性炭的吸附反应场所,强化对元素汞的吸附去除,从而减少燃煤烟气中汞的排放。
在并流吸附反应器和袋式除尘器中,利用活性炭吸附元素汞研究的基础上,建立了袋式除尘器空间活性炭汞吸附模型。利用所建立的模型,讨论了元素汞初始浓度、气布比、温度、碳汞比和颗粒粒径对脱汞效率的影响。模型的建立对利用活性炭喷射技术,控制烟气汞排放的实验研究和工程工艺优化提供了建议。
利用浸渍烧结的方法,制备了负载氧化锰的活性炭纤维(activated carbon fiber, ACF),对负载后材料用TEM、XRD、XPS和FTIR进行了表征,结果表明氧化锰在ACF表面分散良好,颗粒粒径在50nm左右。ACF表面氧化锰的形式为MnO和MnO2。负载后的ACF表面C-OH、C=O、COOH的含量增加。利用负载后材料进行了吸附元素汞的实验,研究结果表明：负载后的ACF吸附汞的穿透时间大大延长。浸渍液浓度对氧化锰的负载量有明显影响,锰负载量为6.7at.%,对汞的去除效率最佳。在150℃时,负载氧化锰后的ACF对元素汞表现出良好的吸附性能。
研究表明活性炭在袋式除尘器中对元素汞的吸附为物理吸附,所建立的吸附模型可以预测操作参数对活性炭吸附元素汞的影响。制备的负载氧化锰的活性炭纤维新型过滤材料对元素汞的吸附为化学吸附,促进了对元素汞的吸附去除。本研究对利用袋式除尘器对烟气中元素汞的去除具有工程指导意义。
Mercury is one of the trace elements in the presence of coal, and it is emitted into the environment with the flue gas in the process of coal combustion. Because of its bioaccumulation and physiological toxicity, mercury pollution control is raised more attention. Mercury pollution caused by coal combustion, has been one of the major environmental problems in China, due to the coal-dominated energy structure. The research on mercury pollution controls technology has been actively carrying out by relevant government departments and scholars. This research is focused on elemental mercury removed by activated carbon in fabric filter, with the support of the National High Technology Research and Development Program (No:2008AA05Z305).
The situation of coal consumption and mercury content in our country was described, the migration and transformation of mercury in the whole process of coal combustion was also explained. The factors affecting on elemental mercury removal by activated carbon both in entrained-flow adsorption reactor and fabric filter were studied, the mercury removal efficiency of dust cake on filter surface was analyzed in detail. The model of mercury sorption by activated carbon in the chamber of filter was established. The load of manganese oxide on activated carbon fiber was prepared and characterized, and the removal capacity of elemental mercury was studied.
The elemental mercury removal capability in the entrained-flow adsorption reactor was investigated using activated carbon as adsorbent. The results showed that:the higher the adsorption temperature, the lower the elemental mercury removal efficiency. When the temperature were at 80℃、120℃、and 150℃, the elemental mercury removal efficiency of activated carbon were reached 46.3%、44.0% and 40.0% respectively。The mercury removal efficiency increases with the C/Hg ratio (mass ratio of injected carbon to mercury) increases, the mercury removal efficiency were 31.3%,34.7%、40.0%, under the C/Hg ratio at 4000,6000 and 8000 respectively
The elemental mercury removal capability in fabric filter was investigated using activated carbon as adsorbent. The total amount of Hg0 adsorption in the fabric filter can be divided into two parts, the amount of Hg0 adsorbed by the activated carbon collected on the filter surface, and the rest removed by the activated carbon somewhere inside the fabric filter. The elemental mercury removal efficiency of fabric filter in the presence of dust cake on the filter surface was investigated in detail. The results showed that:the elemental mercury removal efficiency was significantly improved with the C/Hg ratio increases. The mercury removal efficiency of the activated carbon inside the fabric filter was 30.4%、34.6%、40.3%, under the C/Hg ratio at 4000、6000 and 8000 respectively. But, the mercury removal efficiency of the activated carbon particles collected on the filter surface only reached 3.65%、3.20%、3.66% respectively, The chamber of filter made a major contribution to the mercury removal efficiency, and the dust cake is only a small part of the role. The change of C/Hg ratio has little effect on the elemental mercury removal of the dust cake. Fabric filter can be used as activated carbon adsorption reaction sites, for reducing mercury emissions from coal-fired flue gas.
Based on the results of elemental mercury removal by activated carbon in the entrained-flow reactor and fabric filter, the model of mercury sorption by activated carbon in the chamber of filter was established. The factors affecting the elemental mercury adsorption on activated carbon were discussed, such as:C/Hg ratio, particle diameter, flue-gas temperature, flue-gas velocity, mercury concentration, using the present adsorption model.
The manganese oxide was loaded on the activated carbon fiber (ACF) by impregnating and sintering. The samples of ACF were characterized before and after loading, using TEM、XPS、XRD and FTIR. The results show that manganese oxide was well dispersed on the surface of ACF. The particle diameter was about 50nm. The presence of manganese form was MnO and MnO2. The amount of C-OH、C=O、COOH was increased after loading on the surface of ACF. The adsorption ability of elemental mercury before and after modification was also studied. The breakthrough time was greatly extended after loading. The concentration of impregnating solution had a significant effect on the content of manganese on ACF. The removal efficiency of elemental mercury reached the best when the manganese content on the ACF surface was 6.7at.%. The loaded ACF showed a good adsorption property of elemental mercury at 150℃. The initial concentration of elemental mercury has an impact on the removal efficiency of elemental mercury.
It is shown that elemental mercury adsorption removal by activated carbon in the bag filter is physical adsorption. The adsorption model can predict the impact of operating parameters on the activated carbon adsorption of elemental mercury. The adsorption of elemental mercury by the loaded ACF is chemical adsorption. It can promote the adsorption removal of elemental mercury. This study has a practical significance in the removal of elemental mercury by fabric filter.
引文
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