石灰浆液荷电雾化脱硫的基础理论和试验研究
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摘要
燃煤产生的SO_2已成为生态环境破坏的最大污染源，SO_2污染控制已是急待研究解决的世界性重大课题。燃煤烟气脱硫是目前世界上唯一大规模商业化应用的脱硫技术，其中尤以湿钙法脱硫最为成熟和可靠，是占主导地位的脱硫技术。湿钙法烟气脱硫是气液相际传质及化学反应过程，虽然因其脱硫率高、运行可靠、脱硫剂易得等优势而成为主流技术，但如何进一步改善石灰浆液喷雾效果和SO_2吸收条件，降低投资及运行成本，是该法能否得到普遍推广的关键之一。将高压静电技术引入湿钙法脱硫中是达到上述目的的有效新途径。本文在江苏省高校自然科学基金项目的资助下，针对湿钙法烟气脱硫中使浆液雾滴荷电而产生脱硫增益作用的机理进行深入的理论和试验研究工作。
本文在综合分析当前典型烟气脱硫技术和高压静电雾化技术的基础上，通过石灰浆液静电雾化的机理分析和试验研究，探索石灰浆液流量、充电方式及结构、充电电压与荷电效果的关系，旨在掌握石灰浆液荷电雾化特性；深入分析荷电雾滴吸收SO_2的传质及化学反应动力学机理，初步建立荷电条件下的雾滴脱硫模型；对脱硫塔内部荷电气液两相流动进行质量、动量、能量守恒分析，在考虑传质和反应动力学等因素的情况下，建立石灰浆液荷电雾化脱硫气液两相基本方程及湍流模型；在流场测试的基础上，对脱硫流场进行数值模拟，研究不同条件下的流场特性；设计、建立了石灰浆液荷电雾化脱硫试验装置，对各种不同工况进行脱硫试验，探索石灰浆液荷电雾化脱硫机理。
本文取得的创新性成果如下：
1、首次研究了雾滴带电对SO_2吸收产生影响的机理。认为浆液的雾化使雾滴带上过剩电荷，同时，雾滴在穿越外电场过程中还可能产生非过剩电荷极化带电。雾滴带电主要从三个方面对雾滴表面特性和传质过程产生影响：雾滴形成的偶极矩与气相中极性分子SO_2间的静电力作用，加大气膜扩散速率；雾滴带电引起表面张力及液相SO_2分压下降，增大SO_2吸收的传质推动力；钙离子在雾滴表面的积聚，在促进Ca(OH)_2溶解的同时减小硫分的液相扩散路程，加速传质过程。
2、首次建立了雾滴荷电脱硫模型，为脱硫塔内部流动模型的建立奠定基础。
3、首次在荷电气液两相流动数学模型建立中考虑了SO_2吸收的质量交换和传质推动力等相间作用问题，使模型尽可能贴切地反映脱硫流场的实际情况。
4、首次对三种不同的烟气与浆液雾滴接触方式，进行不同荷电电压、Ca／S、烟气SO_2浓度等参数的对比试验，分别测量系统脱硫率。试验研究表明：脱硫段较短时对进口烟气SO_2浓度的变化比脱硫段较长时敏感；无论是不同的Ca／S或不同荷电电压，雾滴带电都能使脱硫率产生不同程度的提高，并结合理论研究分析了雾滴带电对脱硫效果产生增益作用的机理；明确指出同向流动脱硫率明显优于逆向，雾滴荷电时同向流动脱硫率的增幅也明显优于逆向时的增幅。
本文得到的重要结论如下：
1、明确指出对于感应荷电，荷质比随浆液流量、名义雾化角的增大而增大，但流量增加到一定程度后对提高荷质比的作用不明显，甚至会降低，故从荷电效果看，应尽可能采用较大雾化角和最佳流量值；荷质比随荷电电压的增加而增大，但在本文荷电装置条件下，流量较低时存在最佳电压值；电极放电起始电压随两电极距离H值、名义雾化角和流量的增大而减小；针对荷电雾化脱硫的具体情况得到了环状电极高压静电场场强分布的数学模型。
2、采用PDA和PIV对石灰浆液荷电雾化脱硫流场进行测试，定性、定量研究了荷电对石灰浆液雾滴大小及运动速度的影响规律；定性研究了雾滴荷电时气液两相射流流场发生的变化，该变化将有利于雾滴和烟气的质量、动量和能量交换向全断面拓展，使雾滴和烟气接触在时间上和空间上均得到加强。
3、采用湍流k-ε-k_p模型，首次对石灰浆液荷电雾化脱硫流场进行数值模拟，结果表明：浆液雾滴带电引起流动规律的明显变化，卷吸、旋涡的出现和主流区流速差的降低均有利于烟气与雾滴的混合接触，改善雾滴吸收SO_2的条件；同向流动的流动特点将使其对脱硫效果的改善比逆向流动明显。
4、荷电电压、Ca／S和L／G对脱硫率起着关键性作用，脱硫率随Ca／S的增大而提高，随荷电电压的增加而提高，而且两种情况下提高的幅度同向均比逆向显著；通常增大L／G能提高脱硫率，但过高的浆液流量会影响雾滴荷电效果和雾滴与烟气的接触时间，产生不利因素。
SO_2 generated from coal-burning has become the greatest source of ecological damage to the environment, so SO_2 pollution control has been the worldwide major issue which is the urgent task to be studied and resolved. Flue gas desulphurization is the only large-scale commercial application of desulphurization technology in the world now; especially the wet-calcium-desulphurization is the most mature and reliable desulphurization technology, accounting for the dominant position. Wet calcium flue gas desulphurization is mass transfer and chemical reaction process between gas and liquid. It becomes a mainstream technology for its high rate of desulphurization, reliable operation, and easy to get desulfurizer, etc, but how to further improve the effectiveness of lime slurry spray and SO_2 absorption conditions, reduce investment and operating costs is one of the keys to popularize at large. Introduced here the high-voltage electrostatic technology into wet calcium desulphurization is the effective new way for this purpose. This paper is funded by the University Natural Science Foundation of Jiangsu Province, targeting the wet calcium flue gas desulphurization slurry droplet charged arising from the mechanism of desulphurization gain an in-depth theoretical and experimental research.
Based on the comprehensive analysis of the current typical FGD technology and high-voltage electrostatic atomization technology, and on the basis of lime slurry through electrostatic spray mechanism analysis and pilot studies, this paper explored the relation between the lime slurry flow, charging mode and structure, charging voltage, and the effect of charge, to grasp the lime slurry charge atomization characteristic. Analyzed the mass transfer of droplet SO_2 absorption and chemical reaction kinetics mechanisms, initially established droplet desulphurization model under the charge condition; Analyzed conversation of mass, momentum, energy for internal desulfurizer charge gas and liquid two-phase flow, and established lime slurry atomization desulphurization gas-liquid phase flow basic equation and turbulence model, considering the mass transfer factors and reaction kinetics factors; On the basis of the flow test, theoretically simulated desulphurization flow field, and studied the flow characteristics under different conditions; Designed, established the lime slurry charge atomization tester, experimented in different modes, and explored lime slurry charge atomization desulphurization mechanism.
In this paper, the results of innovative are as follows:
1.First studied the mechanism of droplet charge impacting SO_2 absorption, deemed that the serous spray let the droplet get excess charge, while droplets across the outer electric fields may result the non-excess charge polarization charged. Droplet charged affect the droplets surface characteristics and mass transfer process in three main aspects: droplets formated dipole moment and static force effect of the polar molecule SO_2 in gas, increases gas film diffuse speed; droplet charge arouses the drop of surface tension and liquid SO_2 part pressure, increases mass transfer driving force of SO_2 absorption ; calcium ion accumulates on the droplet surface, promotes the solution of Ca (OH)_2, and shortens the liquid diffuse distance of sulfur, accelerates mass transfer process at the mean time.
2.First established the desulphurization model of droplets charge desulphurization, lies the foundation for the establishment of the internal desulfurizer flow model.
3.First considered the quality exchange of SO_2 absorption and inter-phase mass transfer driving force in the establishment of the mathematical model of charge gas-liquid two-phase flow, to make the model more appropriate to reflect desulphurization flow situation.
4. First comparison tests on three different size droplet contacts with the gas in different charging voltage, Ca / S, flue gas SO_2 concentration parameters, respectively measured the SO_2 removal efficiency of these systems. Experimental study showed: short desulphurization segment is sensitizer to the inlet concentration change of SO_2 than long desulphurization segment; whether Ca / S or charge voltage is different, droplet charge can make desulphurization rate increased in different degrees, and combining theoretical study, analyzed the mechanism of droplet charged produced plus function to desulphurization effect; clearly indicated that the desulphurization rate of flow in the same direction is better than reverse, when the droplet is charged the desulphurization rate amplitude of flow in the same direction is superior to reverse.
In this paper, the important conclusions are as follows:
1.Clearly pointed out that for the induction charge, the charge-to-mass ratio increases with the increasing of slurry flow, the nominal spray angle, but the role of the charge-to-mass ratio is not obvious when flow has increased to some extent, or even lower, so it should adopt the larger spray angle and the optimum flow value as far as possible from the charged electronic effect; The charge-to-mass ratio increases with the increasing voltage, but in this paper ,under this charged electronic equipment conditions , there exists a best voltage value when flow is low; initial electrode discharge voltage decreases when the polar distance H value, the nominal spray angle and flow increases; Found the mathematiac model of the ring electrode high-voltage static electric field intensity distribution .
2. Used PDA and PIV to test lime slurry charge atomization desulphurization flow field, qualitatively and quantitatively researched the law of charge affect lime slurry droplet size and movement velocity; qualitatively researched the changes of gas-liquid two phase flow in the jet when the droplet charged. The changes will be beneficial to the droplet and gas quality, momentum and energy exchange developing to the full-facestrengthened the contact of droplet and gas in time and space.
3.Used turbulence k-ε-k_p model, first theoretically simulated the lime slurrycharge atomization desulphurization flow field, the results showed that: charged slurry droplet caused significant changes of the flow law, entrainment, and the emergence of vortex flow and reduce of velocity of flow difference in the mainstream is propitious to smoke mix and contact with droplet, improve the condition of droplet absorption SO_2, characteristics of flow in the same direction will help to improve the desulphurization effect better than reverse.
4.Charge voltage, Ca / S and L / G play a key role on desulphurization rate. It increases with the accretion of Ca / S, charge voltage, and that in both cases; the same amplitude of increase is more notable than the reverse; usually increasing L/G can enhance the desulphurization rate, but exorbitant slurry flux will affect the effect of droplet charged and the contact time of droplet and flue gas. This is a engender negative factor.
本文在综合分析当前典型烟气脱硫技术和高压静电雾化技术的基础上，通过石灰浆液静电雾化的机理分析和试验研究，探索石灰浆液流量、充电方式及结构、充电电压与荷电效果的关系，旨在掌握石灰浆液荷电雾化特性；深入分析荷电雾滴吸收SO_2的传质及化学反应动力学机理，初步建立荷电条件下的雾滴脱硫模型；对脱硫塔内部荷电气液两相流动进行质量、动量、能量守恒分析，在考虑传质和反应动力学等因素的情况下，建立石灰浆液荷电雾化脱硫气液两相基本方程及湍流模型；在流场测试的基础上，对脱硫流场进行数值模拟，研究不同条件下的流场特性；设计、建立了石灰浆液荷电雾化脱硫试验装置，对各种不同工况进行脱硫试验，探索石灰浆液荷电雾化脱硫机理。
本文取得的创新性成果如下：
1、首次研究了雾滴带电对SO_2吸收产生影响的机理。认为浆液的雾化使雾滴带上过剩电荷，同时，雾滴在穿越外电场过程中还可能产生非过剩电荷极化带电。雾滴带电主要从三个方面对雾滴表面特性和传质过程产生影响：雾滴形成的偶极矩与气相中极性分子SO_2间的静电力作用，加大气膜扩散速率；雾滴带电引起表面张力及液相SO_2分压下降，增大SO_2吸收的传质推动力；钙离子在雾滴表面的积聚，在促进Ca(OH)_2溶解的同时减小硫分的液相扩散路程，加速传质过程。
2、首次建立了雾滴荷电脱硫模型，为脱硫塔内部流动模型的建立奠定基础。
3、首次在荷电气液两相流动数学模型建立中考虑了SO_2吸收的质量交换和传质推动力等相间作用问题，使模型尽可能贴切地反映脱硫流场的实际情况。
4、首次对三种不同的烟气与浆液雾滴接触方式，进行不同荷电电压、Ca／S、烟气SO_2浓度等参数的对比试验，分别测量系统脱硫率。试验研究表明：脱硫段较短时对进口烟气SO_2浓度的变化比脱硫段较长时敏感；无论是不同的Ca／S或不同荷电电压，雾滴带电都能使脱硫率产生不同程度的提高，并结合理论研究分析了雾滴带电对脱硫效果产生增益作用的机理；明确指出同向流动脱硫率明显优于逆向，雾滴荷电时同向流动脱硫率的增幅也明显优于逆向时的增幅。
本文得到的重要结论如下：
1、明确指出对于感应荷电，荷质比随浆液流量、名义雾化角的增大而增大，但流量增加到一定程度后对提高荷质比的作用不明显，甚至会降低，故从荷电效果看，应尽可能采用较大雾化角和最佳流量值；荷质比随荷电电压的增加而增大，但在本文荷电装置条件下，流量较低时存在最佳电压值；电极放电起始电压随两电极距离H值、名义雾化角和流量的增大而减小；针对荷电雾化脱硫的具体情况得到了环状电极高压静电场场强分布的数学模型。
2、采用PDA和PIV对石灰浆液荷电雾化脱硫流场进行测试，定性、定量研究了荷电对石灰浆液雾滴大小及运动速度的影响规律；定性研究了雾滴荷电时气液两相射流流场发生的变化，该变化将有利于雾滴和烟气的质量、动量和能量交换向全断面拓展，使雾滴和烟气接触在时间上和空间上均得到加强。
3、采用湍流k-ε-k_p模型，首次对石灰浆液荷电雾化脱硫流场进行数值模拟，结果表明：浆液雾滴带电引起流动规律的明显变化，卷吸、旋涡的出现和主流区流速差的降低均有利于烟气与雾滴的混合接触，改善雾滴吸收SO_2的条件；同向流动的流动特点将使其对脱硫效果的改善比逆向流动明显。
4、荷电电压、Ca／S和L／G对脱硫率起着关键性作用，脱硫率随Ca／S的增大而提高，随荷电电压的增加而提高，而且两种情况下提高的幅度同向均比逆向显著；通常增大L／G能提高脱硫率，但过高的浆液流量会影响雾滴荷电效果和雾滴与烟气的接触时间，产生不利因素。
SO_2 generated from coal-burning has become the greatest source of ecological damage to the environment, so SO_2 pollution control has been the worldwide major issue which is the urgent task to be studied and resolved. Flue gas desulphurization is the only large-scale commercial application of desulphurization technology in the world now; especially the wet-calcium-desulphurization is the most mature and reliable desulphurization technology, accounting for the dominant position. Wet calcium flue gas desulphurization is mass transfer and chemical reaction process between gas and liquid. It becomes a mainstream technology for its high rate of desulphurization, reliable operation, and easy to get desulfurizer, etc, but how to further improve the effectiveness of lime slurry spray and SO_2 absorption conditions, reduce investment and operating costs is one of the keys to popularize at large. Introduced here the high-voltage electrostatic technology into wet calcium desulphurization is the effective new way for this purpose. This paper is funded by the University Natural Science Foundation of Jiangsu Province, targeting the wet calcium flue gas desulphurization slurry droplet charged arising from the mechanism of desulphurization gain an in-depth theoretical and experimental research.
Based on the comprehensive analysis of the current typical FGD technology and high-voltage electrostatic atomization technology, and on the basis of lime slurry through electrostatic spray mechanism analysis and pilot studies, this paper explored the relation between the lime slurry flow, charging mode and structure, charging voltage, and the effect of charge, to grasp the lime slurry charge atomization characteristic. Analyzed the mass transfer of droplet SO_2 absorption and chemical reaction kinetics mechanisms, initially established droplet desulphurization model under the charge condition; Analyzed conversation of mass, momentum, energy for internal desulfurizer charge gas and liquid two-phase flow, and established lime slurry atomization desulphurization gas-liquid phase flow basic equation and turbulence model, considering the mass transfer factors and reaction kinetics factors; On the basis of the flow test, theoretically simulated desulphurization flow field, and studied the flow characteristics under different conditions; Designed, established the lime slurry charge atomization tester, experimented in different modes, and explored lime slurry charge atomization desulphurization mechanism.
In this paper, the results of innovative are as follows:
1.First studied the mechanism of droplet charge impacting SO_2 absorption, deemed that the serous spray let the droplet get excess charge, while droplets across the outer electric fields may result the non-excess charge polarization charged. Droplet charged affect the droplets surface characteristics and mass transfer process in three main aspects: droplets formated dipole moment and static force effect of the polar molecule SO_2 in gas, increases gas film diffuse speed; droplet charge arouses the drop of surface tension and liquid SO_2 part pressure, increases mass transfer driving force of SO_2 absorption ; calcium ion accumulates on the droplet surface, promotes the solution of Ca (OH)_2, and shortens the liquid diffuse distance of sulfur, accelerates mass transfer process at the mean time.
2.First established the desulphurization model of droplets charge desulphurization, lies the foundation for the establishment of the internal desulfurizer flow model.
3.First considered the quality exchange of SO_2 absorption and inter-phase mass transfer driving force in the establishment of the mathematical model of charge gas-liquid two-phase flow, to make the model more appropriate to reflect desulphurization flow situation.
4. First comparison tests on three different size droplet contacts with the gas in different charging voltage, Ca / S, flue gas SO_2 concentration parameters, respectively measured the SO_2 removal efficiency of these systems. Experimental study showed: short desulphurization segment is sensitizer to the inlet concentration change of SO_2 than long desulphurization segment; whether Ca / S or charge voltage is different, droplet charge can make desulphurization rate increased in different degrees, and combining theoretical study, analyzed the mechanism of droplet charged produced plus function to desulphurization effect; clearly indicated that the desulphurization rate of flow in the same direction is better than reverse, when the droplet is charged the desulphurization rate amplitude of flow in the same direction is superior to reverse.
In this paper, the important conclusions are as follows:
1.Clearly pointed out that for the induction charge, the charge-to-mass ratio increases with the increasing of slurry flow, the nominal spray angle, but the role of the charge-to-mass ratio is not obvious when flow has increased to some extent, or even lower, so it should adopt the larger spray angle and the optimum flow value as far as possible from the charged electronic effect; The charge-to-mass ratio increases with the increasing voltage, but in this paper ,under this charged electronic equipment conditions , there exists a best voltage value when flow is low; initial electrode discharge voltage decreases when the polar distance H value, the nominal spray angle and flow increases; Found the mathematiac model of the ring electrode high-voltage static electric field intensity distribution .
2. Used PDA and PIV to test lime slurry charge atomization desulphurization flow field, qualitatively and quantitatively researched the law of charge affect lime slurry droplet size and movement velocity; qualitatively researched the changes of gas-liquid two phase flow in the jet when the droplet charged. The changes will be beneficial to the droplet and gas quality, momentum and energy exchange developing to the full-facestrengthened the contact of droplet and gas in time and space.
3.Used turbulence k-ε-k_p model, first theoretically simulated the lime slurrycharge atomization desulphurization flow field, the results showed that: charged slurry droplet caused significant changes of the flow law, entrainment, and the emergence of vortex flow and reduce of velocity of flow difference in the mainstream is propitious to smoke mix and contact with droplet, improve the condition of droplet absorption SO_2, characteristics of flow in the same direction will help to improve the desulphurization effect better than reverse.
4.Charge voltage, Ca / S and L / G play a key role on desulphurization rate. It increases with the accretion of Ca / S, charge voltage, and that in both cases; the same amplitude of increase is more notable than the reverse; usually increasing L/G can enhance the desulphurization rate, but exorbitant slurry flux will affect the effect of droplet charged and the contact time of droplet and flue gas. This is a engender negative factor.
引文
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