燃煤电站汞排放环境影响与TAC对烟气零价汞的吸附机理研究
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摘要
汞污染是全球关注的环境问题之一。我国煤炭消耗量巨大,由此引发的燃煤汞排放污染问题日益突出,人们对燃煤汞的排放规律和抑制机理的探索与认识却较少。积极开展燃煤汞排放特性、迁徙转移规律及汞污染防治技术等相关研究,对减少燃煤烟气汞排放及其周边环境影响等具有重要意义。本文针对燃煤汞排放周边影响及汞吸附机制等问题,围绕燃煤电站烟气汞采样分析、汞排放的周边环境影响、活性炭控制烟气汞吸附机理以及NOx、汞污染物协同控制等四个方面开展了深入的研究。
首先,依据燃煤电站的烟气汞特性和干吸附测汞法基本原理,自行设计建立了一套便捷的干吸附形态汞取样测试系统(Flue gas mercury speciation system, FMSS),并与OH、CEM等常规取样测试方法一起对国内3个典型燃煤电站进行了汞排放的对比测试。结果表明,所测燃煤烟气汞浓度介于2.8-14.3μg/m3之间,三种测试方法对同一采样点的总汞测试偏差仅6.7%,在SO2浓度高达1248ppm时,FMSS测得的结果仍可满足70%-130%的锅炉汞平衡要求,这为适合国情的燃煤电站烟气形态汞的便捷取样测试方法建立打下基础。
其次,采用基于汞排放源数据以及气象、地理条件的模型计算,结合周边环境介质的采样分析,应用地统计学的方法系统研究了一2×125MW燃煤电站烟气汞排放的迁徙转移规律及其对局域环境的影响。结果表明周边表层土壤汞含量介于0.045-0.529mg/kg之间,均值0.180mg/kg,与当地土壤背景汞含量相比增加了2.3%；在半径7km的采样区域内,电站周边地表大气中汞的浓度范围为4.3-12.4ng/m3,均值7.0ng/m3,略高于当地背景值(6.7ng/m3)；在高斯扩散与干湿沉降的共同作用下,地表大气汞浓度随着与电站距离的增加总体上呈驼峰形递减的分布规律。
再者,本文进行了基于表面汞形态分析的活性炭吸汞机理研究。采用惰性气氛下高温脱附的方法制备高温脱附活性炭(heat-treated activated carbon, TAC),以消除表面化学官能团与烟气组分的交互影响,在模拟烟气实验台上开展不同烟气组分下TAC对Hg0的吸附实验,并利用XPS、XAFS等先进测试手段对吸汞产物中汞的赋存状态和配位情况进行分析研究。结果表明,TAC对Hg0的吸附并非简单的物理吸附；酸性气体组分下Hg0在TAC上的吸附主要遵循Eley-Rideal反应机理,酸性气体组分在TAC活性反应位上的反应和吸附为氧化吸附Hg0提供了所需的酸性反应基团,TAC则起促进酸性反应基团生成以及汞氧化的催化作用；在本文实验条件下,N2气氛中单一组分HCl、NO2或NO的添加均可使TAC氧化吸附Hg0的效率高达50%以上,而S02仅约20%；酸性气体组分下,02对TAC氧化吸附Hg0具有一定的协同促进作用；与其它酸性气体组分同时存在时,802可通过竞争吸附TAC表面活性位的方式降低TAC对Hg0的吸附性能,且这种现象在H20存在时更为明显。
最后,围绕NOx、汞两种燃煤污染物的协同控制展开了实验研究。在空速8000h-1、烟温80-100℃的实验条件下,活性炭拥有良好的NOx吸附性能,且饱和吸附后,在O2含量低至4%时,活性炭在高效脱汞同时催化氧化NO的效率仍可达55%。基于以上研究结果,本文提出了一种利用活性炭实现对燃煤烟气NOx和汞协同脱除的可行技术途径。
Mercury pollution is one of the global environmental challenges. Problems arising from the release of mercury are increasing in China because of the huge coal consumption. However, the mercury pollution is less known among the public and subsequent affordable strategies for mercury control are still needed. Therefore, there is an urgent need to carry out studies on mercury emission characteristics, mercury transportation pattern, and mercury control technology. To understand the impacts of mercury emission from coal-fired power plants and the adsorption mechanism of mercury, researches were carried out on the measurement of mercury, environmental impacts, mechanism of mercury adsorption on activated carbon and the cooperative control technology.
At first, a set of flue gas mercury speciation system (FMSS) was designed and built to meet the shortage of measurement methods for coal-fired power plants. Field validations and comparison with CEM and OH method were carried out in three different power plants. Results showed that mercury concentrations in the flue gases from coal-fired power plants were in the range of2.8-14.3μg/m3.The deviation of total mercury concentrations measured by three methods in the same flue gas was6.7%. The mercury concentration measured by FMSS still met the70%-130%requirement in the mercury balance of boiler even in the flue gas with1248ppm SO2, and thus suitable for convenient mercury measurement in coal-fired flue gases.
Secondly, in combination with the emission source, local meteorological and geographical conditions, model calculations were carried out and samples of soil and air were collected and analyzed to evaluate the environmental effect of mercury emission from a typical coal-fired power plant. Spatial distribution of mercury in soil and air around a2×125MW power plant were investigated using geostatistics techniques. It was found that mercury levels in soil samples were in the range of0.045-0.529mg/kg with an average of0.180mg/kg. In comparison with the local soil background, the average mercury content of nearby soil increased by2.3%. Within the7km radius areas of sample collection, mercury concentrations in air samples varied from4.3to12.4ng/m3with an average of7.0ng/m3, slightly higher than the local background of6.7ng/m3. As the result of Gaussian diffusion together with physical deposition, mercury concentration in air samples decreased in general with the increase of the distance from the power plant, except for a peak value at certain distance downwind the chimney.
Furthermore, absorption mechanisms of mercury on activated carbon were studied based on the morphological analysis of adsorbed mercury on activated carbon surface. Surface functional groups (SFGs) on AC sorbents were removed through heat treatment under the protection of argon (Ar). The Hg0adsorption behavior of heat-treated activated carbon (TAC) when subjected to various synthetic gases was studied. The use of TAC was to avoid the complicated interaction between SFGs and flue gas components. The adsorbed residues were then characterized by XPS and XAFS to investigate the existing state of mercury and its coordination properties. We found that the Hg0adsorption on AC was not simply a process of physical adsorption. Acid gas components enhance Hg0capture on TAC mainly through Eley-Rideal reaction mechanism. The adsorption of acid gas component and subsequent formation of acidic reactive groups on TAC provided activated sites for Hg0sorption, while TAC served as a catalyst for the formation of acidic reactive groups and the oxidization of mercury. Under the experimental conditions of our study, the addition of single acid component (HC1, NO2or NO) to the pure N2can generate higher Hg0capture efficiency larger than50%, while it was only20%when SO2was added. O2exhibits a synergistic effect on the enhancement of Hg0oxidation and capture when acid gases are present in baseline gases. When co-existed with other acid gas components, SO2can inhibit the adsorption of mercury through competition for the same active site on TAC. The addition of water vapor promoted the adsorption of SO2on TAC further.
Finally, experimental studies were carried out on the cooperative control of NOx and Hg0, which are the two major pollutants from coal burning. Activated carbon can adsorb NOx very well under the temperature range of80-100℃with a space flow rate of8000h-1. After NOx adsorption reached saturation, the activated carbon still can remove mercury efficiently and simultaneously catalyze the oxidation of NO up to55%in the presence of only4%O2. Therefore, an economical approach that used activated carbon for the simultaneous removal of NOx and mercury in flue gas was developed in this paper.
首先,依据燃煤电站的烟气汞特性和干吸附测汞法基本原理,自行设计建立了一套便捷的干吸附形态汞取样测试系统(Flue gas mercury speciation system, FMSS),并与OH、CEM等常规取样测试方法一起对国内3个典型燃煤电站进行了汞排放的对比测试。结果表明,所测燃煤烟气汞浓度介于2.8-14.3μg/m3之间,三种测试方法对同一采样点的总汞测试偏差仅6.7%,在SO2浓度高达1248ppm时,FMSS测得的结果仍可满足70%-130%的锅炉汞平衡要求,这为适合国情的燃煤电站烟气形态汞的便捷取样测试方法建立打下基础。
其次,采用基于汞排放源数据以及气象、地理条件的模型计算,结合周边环境介质的采样分析,应用地统计学的方法系统研究了一2×125MW燃煤电站烟气汞排放的迁徙转移规律及其对局域环境的影响。结果表明周边表层土壤汞含量介于0.045-0.529mg/kg之间,均值0.180mg/kg,与当地土壤背景汞含量相比增加了2.3%；在半径7km的采样区域内,电站周边地表大气中汞的浓度范围为4.3-12.4ng/m3,均值7.0ng/m3,略高于当地背景值(6.7ng/m3)；在高斯扩散与干湿沉降的共同作用下,地表大气汞浓度随着与电站距离的增加总体上呈驼峰形递减的分布规律。
再者,本文进行了基于表面汞形态分析的活性炭吸汞机理研究。采用惰性气氛下高温脱附的方法制备高温脱附活性炭(heat-treated activated carbon, TAC),以消除表面化学官能团与烟气组分的交互影响,在模拟烟气实验台上开展不同烟气组分下TAC对Hg0的吸附实验,并利用XPS、XAFS等先进测试手段对吸汞产物中汞的赋存状态和配位情况进行分析研究。结果表明,TAC对Hg0的吸附并非简单的物理吸附；酸性气体组分下Hg0在TAC上的吸附主要遵循Eley-Rideal反应机理,酸性气体组分在TAC活性反应位上的反应和吸附为氧化吸附Hg0提供了所需的酸性反应基团,TAC则起促进酸性反应基团生成以及汞氧化的催化作用；在本文实验条件下,N2气氛中单一组分HCl、NO2或NO的添加均可使TAC氧化吸附Hg0的效率高达50%以上,而S02仅约20%；酸性气体组分下,02对TAC氧化吸附Hg0具有一定的协同促进作用；与其它酸性气体组分同时存在时,802可通过竞争吸附TAC表面活性位的方式降低TAC对Hg0的吸附性能,且这种现象在H20存在时更为明显。
最后,围绕NOx、汞两种燃煤污染物的协同控制展开了实验研究。在空速8000h-1、烟温80-100℃的实验条件下,活性炭拥有良好的NOx吸附性能,且饱和吸附后,在O2含量低至4%时,活性炭在高效脱汞同时催化氧化NO的效率仍可达55%。基于以上研究结果,本文提出了一种利用活性炭实现对燃煤烟气NOx和汞协同脱除的可行技术途径。
Mercury pollution is one of the global environmental challenges. Problems arising from the release of mercury are increasing in China because of the huge coal consumption. However, the mercury pollution is less known among the public and subsequent affordable strategies for mercury control are still needed. Therefore, there is an urgent need to carry out studies on mercury emission characteristics, mercury transportation pattern, and mercury control technology. To understand the impacts of mercury emission from coal-fired power plants and the adsorption mechanism of mercury, researches were carried out on the measurement of mercury, environmental impacts, mechanism of mercury adsorption on activated carbon and the cooperative control technology.
At first, a set of flue gas mercury speciation system (FMSS) was designed and built to meet the shortage of measurement methods for coal-fired power plants. Field validations and comparison with CEM and OH method were carried out in three different power plants. Results showed that mercury concentrations in the flue gases from coal-fired power plants were in the range of2.8-14.3μg/m3.The deviation of total mercury concentrations measured by three methods in the same flue gas was6.7%. The mercury concentration measured by FMSS still met the70%-130%requirement in the mercury balance of boiler even in the flue gas with1248ppm SO2, and thus suitable for convenient mercury measurement in coal-fired flue gases.
Secondly, in combination with the emission source, local meteorological and geographical conditions, model calculations were carried out and samples of soil and air were collected and analyzed to evaluate the environmental effect of mercury emission from a typical coal-fired power plant. Spatial distribution of mercury in soil and air around a2×125MW power plant were investigated using geostatistics techniques. It was found that mercury levels in soil samples were in the range of0.045-0.529mg/kg with an average of0.180mg/kg. In comparison with the local soil background, the average mercury content of nearby soil increased by2.3%. Within the7km radius areas of sample collection, mercury concentrations in air samples varied from4.3to12.4ng/m3with an average of7.0ng/m3, slightly higher than the local background of6.7ng/m3. As the result of Gaussian diffusion together with physical deposition, mercury concentration in air samples decreased in general with the increase of the distance from the power plant, except for a peak value at certain distance downwind the chimney.
Furthermore, absorption mechanisms of mercury on activated carbon were studied based on the morphological analysis of adsorbed mercury on activated carbon surface. Surface functional groups (SFGs) on AC sorbents were removed through heat treatment under the protection of argon (Ar). The Hg0adsorption behavior of heat-treated activated carbon (TAC) when subjected to various synthetic gases was studied. The use of TAC was to avoid the complicated interaction between SFGs and flue gas components. The adsorbed residues were then characterized by XPS and XAFS to investigate the existing state of mercury and its coordination properties. We found that the Hg0adsorption on AC was not simply a process of physical adsorption. Acid gas components enhance Hg0capture on TAC mainly through Eley-Rideal reaction mechanism. The adsorption of acid gas component and subsequent formation of acidic reactive groups on TAC provided activated sites for Hg0sorption, while TAC served as a catalyst for the formation of acidic reactive groups and the oxidization of mercury. Under the experimental conditions of our study, the addition of single acid component (HC1, NO2or NO) to the pure N2can generate higher Hg0capture efficiency larger than50%, while it was only20%when SO2was added. O2exhibits a synergistic effect on the enhancement of Hg0oxidation and capture when acid gases are present in baseline gases. When co-existed with other acid gas components, SO2can inhibit the adsorption of mercury through competition for the same active site on TAC. The addition of water vapor promoted the adsorption of SO2on TAC further.
Finally, experimental studies were carried out on the cooperative control of NOx and Hg0, which are the two major pollutants from coal burning. Activated carbon can adsorb NOx very well under the temperature range of80-100℃with a space flow rate of8000h-1. After NOx adsorption reached saturation, the activated carbon still can remove mercury efficiently and simultaneously catalyze the oxidation of NO up to55%in the presence of only4%O2. Therefore, an economical approach that used activated carbon for the simultaneous removal of NOx and mercury in flue gas was developed in this paper.
引文
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