石灰石活性和塔内流场对湿法烟气脱硫效率的影响研究
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摘要
随着经济和社会的发展，燃煤造成的SO_2及NOx污染日益严重。在目前的烟气脱硫工艺中，石灰石-石膏湿法烟气脱硫工艺由于具有技术成熟、运行可靠、脱硫效率高、吸收剂来源丰富、价格低廉等优点，获得了广泛的应用。在石灰石-石膏湿法烟气脱硫系统中，作为吸收剂的石灰石的活性以及脱硫塔内的流场分布对SO_2的吸收有着重要影响。针对国外烟气脱硫工艺在中国运行过程中出现的问题，以提高脱硫效率和系统运行的经济性以及实现以湿法烟气脱硫工艺为基础的多种污染物同时脱除为目的，本文对石灰石的活性、脱硫塔内气液传质的优化以及石灰石浆液吸收NO_2的机理进行了研究。
通过定pH值滴定法考察了pH值、温度、粒径分布、石膏、飞灰、Al~(3+)、F、NO_3~-等因素对石灰石溶解过程的影响。较低的pH值、较高的反应温度和较小的石灰石粒径分布有利于石灰石的溶解；石膏、飞灰对石灰石的溶解有轻微的抑制作用；Al~(3+)与F~-形成的络合物则会严重抑制石灰石的溶解。
为考察石灰石成分对其脱硫能力的影响，测试了42种不同产地的石灰石样品的脱硫能力；系统分析了石灰石的化学成分，包括CaO、MgO、Fe_2O_3、Al_2O_3、SiO_2、烧失量等对其脱硫能力的影响。结果表明：CaO和MgO含量是影响石灰石脱硫能力的关键因素；SiO_2和Fe_2O_3含量对石灰石的脱硫能力也有一定影响。此外,XRD结果表明，石灰石脱硫能力与方解石的结晶程度密切相关，白云石相的存在会严重抑制石灰石的溶解。
为考察石灰石的品质对SO_2吸收的影响，基于气体吸收的双膜理论，建立了通过石灰石品质和粒径分布来预测喷淋塔脱硫性能的数学模型，并进行了相应的试验研究。该模型中，石灰石种类的不同对SO_2吸收的影响通过石灰石溶解的表面反应速率常数来解释；对于同种石灰石来说，粒径分布越小，比表面积越大，溶解越快，越有利于SO_2的吸收。
通过安装气液传质强化构件，对湿法烟气脱硫喷淋塔内的气液传质进行了优化试验研究及CFD模拟。结果表明，气液传质强化构件能够防止烟气沿塔壁逃逸，整流气相流场，强化气液两相在吸收区的混合，有利于SO_2的吸收。通流截面一定时，喷淋区压降和脱硫效率随构件与水平面夹角的增大而增大；构件与水平面夹角一定时，喷淋区压降和脱硫效率随通流截面的增大而减小。
利用双搅拌釜反应器研究了NO_2在石灰石浆液中的吸收过程；考察了各种因素如石灰石浆液浓度、反应温度、石灰石颗粒的粒径分布、搅拌速率、NO_2入口浓度及烟气中的含氧量等因素对NO_2吸收速率的影响。结果表明，在NO_2的吸收过程中，石灰石的溶解具有重要影响。NO_2的吸收速率随着搅拌速率、NO_2入口浓度和烟气中含氧量的升高而升高，而且较低的反应温度有利于NO_2的吸收。在喷淋塔内，NO_2脱除效率随烟气停留时间的延长而升高。
With the development of economy and society, the environment is badly polluted by SO_2 and NOx from coal-fired boilers. At Present limestone-gypsum wet flue gas desulfurization technology is being widely applied all over the world because of its advantages: sophisticated technology and reliable operation, high desulfurization efficiency, widespread and cheap absorbent. In a WFGD system, the reactivity of limestone and the flow field distribution in the scrubber are of great effect on SO_2 absorption. According to the problems during the operation of foreign desulfurization process in China, in order to improve the SO_2 removal efficiency and operation economical efficiency of WFGD system and simultaneous removal SO_2 and NO_x through wet flue gas desulfurization process, the reactivity of limestone, optimization of the gas-liquid mass transfer in the scrubber and the absorption mechanism NO_2 by limestone slurry are studied in this dissertation.
The impact of pH value, temperature, particle size distribution, gypsum, fly ash, Al~(3+), F~- and NO_3~- on the dissolution of limestone was investigated by pH-stat method. It seems that lower pH value, higher reaction temperature and smaller particle size are favorable to limestone dissolution. Gypsum or fly ash has a little inhibition effect on limestone dissolution and the aluminum/fluoride complexes (AlFx) inhibit the dissolution of limestone seriously.
To study the relation between limestone chemical components and its desulfurization capacity, the desulfurization capacity of 42 kinds of limestone from different sources was tested. The correlation between limestone desulfurization capacity and its chemical components, including CaO, MgO, Al_2O_3, Fe_2O_3, SiO_2 and ignition loss was systemically analyzed to identify the key component which influenced the desulfurization capacity. The results showed that the content of CaO and MgO was the key factor influenced the desulfurization capacity of limestone. And the content of SiO_2 and Fe_2O_3 had some effect on limestone desulfurization capacity.In addition, as is shown in the XRD results, the desulfurization capacity of limestone was closely related to the crystallinity of calcite and the existence of dolomite would inhibit the dissolution seriously.
In order to investigate the effects of limestone quality on SO_2 removal, the effects of limestone type and particle size distribution on SO_2 removal were studied by numerical model based on the two film theory of gas absorption and experimental method.The dissolution surface reaction rate constant variations accounted for differences between limestone types. As for the same kind of limestone, smaller particles had larger specific area and dissolved at a greater rate, thus could absorb more SO_2.
By installing the gas-liquid mass transfer strengthening component in the spray scrubber for wet flue gas desulfurization, the mass transfer in it was studied by experimental and CFD simulation method. As can be seen from the results, flue gas can be prevented from escaping along scrubber wall by the component, flue gas flow field is rectified and the mixture of gas and liquid phase are strengthened too, they are all favorable to the absorption of SO_2. In addition, at a definite flow-through section, the pressure drop and SO_2 removal efficiency of the scrubber increase with the increase of the angle between the component and horizontal plane; and at a definite angle between the component and horizontal plane, the pressure drop and SO_2 removal efficiency drop with the increase of flow-through section.
An experimental study on the absorption of low concentration nitrogen dioxide into limestone slurries in a stirred tank reactor with a plane gas-liquid interface has been performed. The absorption rates under various conditions such as limestone slurry concentration, reaction temperature, limestone particle size distribution; stirred speed, NO_2 inlet concentration and O_2 content in the simulated flue gas were measured and the absorption processes had been discussed. As can be seen from the results, limestone dissolution has a great effect on nitrogen dioxide absorption.NO_2 absorption rate increases with the increase of stirred speed, NO_2 inlet concentration and O_2 content in the flue gas, and lower reaction temperature is favorable to NO2 absorption. And NO_2 removal efficiency increases with increasing flue gas residence time in spray scrubber.
通过定pH值滴定法考察了pH值、温度、粒径分布、石膏、飞灰、Al~(3+)、F、NO_3~-等因素对石灰石溶解过程的影响。较低的pH值、较高的反应温度和较小的石灰石粒径分布有利于石灰石的溶解；石膏、飞灰对石灰石的溶解有轻微的抑制作用；Al~(3+)与F~-形成的络合物则会严重抑制石灰石的溶解。
为考察石灰石成分对其脱硫能力的影响，测试了42种不同产地的石灰石样品的脱硫能力；系统分析了石灰石的化学成分，包括CaO、MgO、Fe_2O_3、Al_2O_3、SiO_2、烧失量等对其脱硫能力的影响。结果表明：CaO和MgO含量是影响石灰石脱硫能力的关键因素；SiO_2和Fe_2O_3含量对石灰石的脱硫能力也有一定影响。此外,XRD结果表明，石灰石脱硫能力与方解石的结晶程度密切相关，白云石相的存在会严重抑制石灰石的溶解。
为考察石灰石的品质对SO_2吸收的影响，基于气体吸收的双膜理论，建立了通过石灰石品质和粒径分布来预测喷淋塔脱硫性能的数学模型，并进行了相应的试验研究。该模型中，石灰石种类的不同对SO_2吸收的影响通过石灰石溶解的表面反应速率常数来解释；对于同种石灰石来说，粒径分布越小，比表面积越大，溶解越快，越有利于SO_2的吸收。
通过安装气液传质强化构件，对湿法烟气脱硫喷淋塔内的气液传质进行了优化试验研究及CFD模拟。结果表明，气液传质强化构件能够防止烟气沿塔壁逃逸，整流气相流场，强化气液两相在吸收区的混合，有利于SO_2的吸收。通流截面一定时，喷淋区压降和脱硫效率随构件与水平面夹角的增大而增大；构件与水平面夹角一定时，喷淋区压降和脱硫效率随通流截面的增大而减小。
利用双搅拌釜反应器研究了NO_2在石灰石浆液中的吸收过程；考察了各种因素如石灰石浆液浓度、反应温度、石灰石颗粒的粒径分布、搅拌速率、NO_2入口浓度及烟气中的含氧量等因素对NO_2吸收速率的影响。结果表明，在NO_2的吸收过程中，石灰石的溶解具有重要影响。NO_2的吸收速率随着搅拌速率、NO_2入口浓度和烟气中含氧量的升高而升高，而且较低的反应温度有利于NO_2的吸收。在喷淋塔内，NO_2脱除效率随烟气停留时间的延长而升高。
With the development of economy and society, the environment is badly polluted by SO_2 and NOx from coal-fired boilers. At Present limestone-gypsum wet flue gas desulfurization technology is being widely applied all over the world because of its advantages: sophisticated technology and reliable operation, high desulfurization efficiency, widespread and cheap absorbent. In a WFGD system, the reactivity of limestone and the flow field distribution in the scrubber are of great effect on SO_2 absorption. According to the problems during the operation of foreign desulfurization process in China, in order to improve the SO_2 removal efficiency and operation economical efficiency of WFGD system and simultaneous removal SO_2 and NO_x through wet flue gas desulfurization process, the reactivity of limestone, optimization of the gas-liquid mass transfer in the scrubber and the absorption mechanism NO_2 by limestone slurry are studied in this dissertation.
The impact of pH value, temperature, particle size distribution, gypsum, fly ash, Al~(3+), F~- and NO_3~- on the dissolution of limestone was investigated by pH-stat method. It seems that lower pH value, higher reaction temperature and smaller particle size are favorable to limestone dissolution. Gypsum or fly ash has a little inhibition effect on limestone dissolution and the aluminum/fluoride complexes (AlFx) inhibit the dissolution of limestone seriously.
To study the relation between limestone chemical components and its desulfurization capacity, the desulfurization capacity of 42 kinds of limestone from different sources was tested. The correlation between limestone desulfurization capacity and its chemical components, including CaO, MgO, Al_2O_3, Fe_2O_3, SiO_2 and ignition loss was systemically analyzed to identify the key component which influenced the desulfurization capacity. The results showed that the content of CaO and MgO was the key factor influenced the desulfurization capacity of limestone. And the content of SiO_2 and Fe_2O_3 had some effect on limestone desulfurization capacity.In addition, as is shown in the XRD results, the desulfurization capacity of limestone was closely related to the crystallinity of calcite and the existence of dolomite would inhibit the dissolution seriously.
In order to investigate the effects of limestone quality on SO_2 removal, the effects of limestone type and particle size distribution on SO_2 removal were studied by numerical model based on the two film theory of gas absorption and experimental method.The dissolution surface reaction rate constant variations accounted for differences between limestone types. As for the same kind of limestone, smaller particles had larger specific area and dissolved at a greater rate, thus could absorb more SO_2.
By installing the gas-liquid mass transfer strengthening component in the spray scrubber for wet flue gas desulfurization, the mass transfer in it was studied by experimental and CFD simulation method. As can be seen from the results, flue gas can be prevented from escaping along scrubber wall by the component, flue gas flow field is rectified and the mixture of gas and liquid phase are strengthened too, they are all favorable to the absorption of SO_2. In addition, at a definite flow-through section, the pressure drop and SO_2 removal efficiency of the scrubber increase with the increase of the angle between the component and horizontal plane; and at a definite angle between the component and horizontal plane, the pressure drop and SO_2 removal efficiency drop with the increase of flow-through section.
An experimental study on the absorption of low concentration nitrogen dioxide into limestone slurries in a stirred tank reactor with a plane gas-liquid interface has been performed. The absorption rates under various conditions such as limestone slurry concentration, reaction temperature, limestone particle size distribution; stirred speed, NO_2 inlet concentration and O_2 content in the simulated flue gas were measured and the absorption processes had been discussed. As can be seen from the results, limestone dissolution has a great effect on nitrogen dioxide absorption.NO_2 absorption rate increases with the increase of stirred speed, NO_2 inlet concentration and O_2 content in the flue gas, and lower reaction temperature is favorable to NO2 absorption. And NO_2 removal efficiency increases with increasing flue gas residence time in spray scrubber.
引文
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