窄间隙气体放电烟气脱硫资源化研究
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摘要
我国的能源结构以煤炭为主，燃煤型SO_2污染已成为我国大气污染的主要特征，因此对二氧化硫污染的治理已经刻不容缓。本文针对我国目前严峻的SO_2污染形势，而传统的烟气脱硫技术存在着运行成本高；产生大量的污水需要处理；典型的非平衡等离子体法又需要外加NH_3、电子能量低等问题，结合国家自然科学基金重点资助项目“高气压下强电场电离气体的方法及其应用的基础研究”(项目编号：60031001)，提出了以窄间隙强电场电离气体放电产生高浓度羟基自由基氧化脱除烟气中SO_2的方法进行烟气脱硫，为SO_2污染的治理提供了一条新途径。
采用窄间隙强电场电离放电技术，可以在等离子体反应器的反应腔体内形成放电电场强度高达400Td以上的强电场，使电子获得的平均能量大于10eV，电子密度大于10~(14)／cm~3，电离占空比达到2％，足以满足等离子体化学反应所需的能量要求，从而将烟气中的H_2O、O_2(H_2O、O_2气体分子的电离能分别为12.6eV、12.5eV)等气体分子电离离解形成高浓度的OH·、e_(aq)~—等氧化自由基，直接在气相中瞬间将SO_2氧化为H_2SO_4以将其脱除。
通过对实验系统的混气方式及气体的加湿方法进行改进，建立了一套新的实验系统，并在此基础上考察了各种参数对SO_2脱除率的影响，由实验结果可知提高电源激励电压、激励频率、放电功率、含水量、含氧量或降低SO_2初始浓度、模拟烟气总气量，减小放电间隙都能提高SO_2的脱除率。通过比较不同放电面积等离子体反应器所得的实验结果后可知，等离子体反应器放电面积的变化不会影响SO_2脱除率的变化规律。文中还对模拟烟气中的含水量及含氧量对SO_2脱除率的影响强度进行了对比，得出含水量对SO_2脱除率的影响强于含氧量的影响。实验结果表面，当等离子体反应器放电间隙为0.64mm，电源激励电压为2600V，激励频率为5000Hz，模拟烟气总流量为0.1m~3／h，含氧量为21％，含水量为1.44％，SO_2初始浓度为400ppm时，SO_2脱除率可达到99％，满足了对SO_2治理的要求，说明窄间隙强电场电离气体放电是一种绿色有效的脱硫新途径。
The coal is the main energy sources in our country. SO_2 pollution deriving from burning coal has been the main characteristic of atmospheric pollution in our country. Therefore the treatment of SO_2 pollution must been carried out as soon as possible. For typical desulfuration technologies have many problems such as high cost, waste water producing, NH3 adding, low electron energy, etc, the method of desulfuration using OH radicals produced by strong electric field ionization discharge is presented in this paper, which is based on the key NSFC project "Studies of Method and Application of Gas Molecules Ionized with Strong Electric at High Pressure Field" (No.: 60031001). It is a kind of new desulfuration technology.
Using the narrow gap strong electric field ionization discharge technology, the strong electric field whose intensity is high up to 400Td is formed in the chamber of the plasma reactor. Thanks to the high electric field, a great number of energetic electrons are produced whose electron mean energy, electron density and fractional active volume are 10eV, 10~(14)/cm~3 and 2%, respectively. The energetic electrons can provide enough energy for plasma chemical reactions. They can ionize H_2O and O_2 to form OH 、 e_(aq)-radicals and SO_2 can be removed by the oxidization of SO_2 to H2SO4 by these radicals.
The new experimental system is established. The findings are the SO_2 removal efficiency can be enhanced by increasing the excitation voltage, excitation frequency, excitation power, H_2O concentration, O_2 concentration or decreasing SO_2 initial concentration, simulative flue gas total flux and discharge gap. The changing rule of desulfuration efficiency will not be changed if the discharge area of plasma reactor is changed. In this paper, the comparison of effect intensity on desulfuration efficiency of water and oxygen concentration of simulation flue gas is also made, and the conclusion is drawn that the effect of water concentration of gas on desulfuration efficiency is larger than that oxygen concentration do. The experimental results show when the discharge gap, excitation voltage, excitation frequency, simulative flue gas total flux, O_2
采用窄间隙强电场电离放电技术，可以在等离子体反应器的反应腔体内形成放电电场强度高达400Td以上的强电场，使电子获得的平均能量大于10eV，电子密度大于10~(14)／cm~3，电离占空比达到2％，足以满足等离子体化学反应所需的能量要求，从而将烟气中的H_2O、O_2(H_2O、O_2气体分子的电离能分别为12.6eV、12.5eV)等气体分子电离离解形成高浓度的OH·、e_(aq)~—等氧化自由基，直接在气相中瞬间将SO_2氧化为H_2SO_4以将其脱除。
通过对实验系统的混气方式及气体的加湿方法进行改进，建立了一套新的实验系统，并在此基础上考察了各种参数对SO_2脱除率的影响，由实验结果可知提高电源激励电压、激励频率、放电功率、含水量、含氧量或降低SO_2初始浓度、模拟烟气总气量，减小放电间隙都能提高SO_2的脱除率。通过比较不同放电面积等离子体反应器所得的实验结果后可知，等离子体反应器放电面积的变化不会影响SO_2脱除率的变化规律。文中还对模拟烟气中的含水量及含氧量对SO_2脱除率的影响强度进行了对比，得出含水量对SO_2脱除率的影响强于含氧量的影响。实验结果表面，当等离子体反应器放电间隙为0.64mm，电源激励电压为2600V，激励频率为5000Hz，模拟烟气总流量为0.1m~3／h，含氧量为21％，含水量为1.44％，SO_2初始浓度为400ppm时，SO_2脱除率可达到99％，满足了对SO_2治理的要求，说明窄间隙强电场电离气体放电是一种绿色有效的脱硫新途径。
The coal is the main energy sources in our country. SO_2 pollution deriving from burning coal has been the main characteristic of atmospheric pollution in our country. Therefore the treatment of SO_2 pollution must been carried out as soon as possible. For typical desulfuration technologies have many problems such as high cost, waste water producing, NH3 adding, low electron energy, etc, the method of desulfuration using OH radicals produced by strong electric field ionization discharge is presented in this paper, which is based on the key NSFC project "Studies of Method and Application of Gas Molecules Ionized with Strong Electric at High Pressure Field" (No.: 60031001). It is a kind of new desulfuration technology.
Using the narrow gap strong electric field ionization discharge technology, the strong electric field whose intensity is high up to 400Td is formed in the chamber of the plasma reactor. Thanks to the high electric field, a great number of energetic electrons are produced whose electron mean energy, electron density and fractional active volume are 10eV, 10~(14)/cm~3 and 2%, respectively. The energetic electrons can provide enough energy for plasma chemical reactions. They can ionize H_2O and O_2 to form OH 、 e_(aq)-radicals and SO_2 can be removed by the oxidization of SO_2 to H2SO4 by these radicals.
The new experimental system is established. The findings are the SO_2 removal efficiency can be enhanced by increasing the excitation voltage, excitation frequency, excitation power, H_2O concentration, O_2 concentration or decreasing SO_2 initial concentration, simulative flue gas total flux and discharge gap. The changing rule of desulfuration efficiency will not be changed if the discharge area of plasma reactor is changed. In this paper, the comparison of effect intensity on desulfuration efficiency of water and oxygen concentration of simulation flue gas is also made, and the conclusion is drawn that the effect of water concentration of gas on desulfuration efficiency is larger than that oxygen concentration do. The experimental results show when the discharge gap, excitation voltage, excitation frequency, simulative flue gas total flux, O_2
引文
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[17] Paur H R，Jordan s，Aerosol Formation in the Electron Beam Dry Scrubbing Process，Radiat Phys Chem，1988，31(3)：9～13
[18] Okihiro Tokunaga.Electron Beam Irradiation Technology for Purification of Flue Gas.Journal of the Institute of the Institute of Electrostatics Japan.1995,19(4):296～300
[19] E A Filimonova,R H Amirrov, H T Kim et al. Comparative Modeling of NO_x and SO_2 Removal from Pollutant Gases Using Pulsed-Corona and Silent Discharges, J. Plys. D; Appl. Phys, 2000,33:1716～1727
[20] 陈亚非，张奇兴，电子束烟气脱硫若干问题探讨，中国电力，2000，33(7)：78～80
[21] 邰德荣，韩宾兵，成都电厂电子束烟气脱硫示范工程，中国电力，1998，31(11)：42～47
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[23] T Urabe, Y Wu, S Masuda et al, Experimental Studies on NO_x and SO_2 Removal by Pulse Corona Discharge, Proc Inst Electrostatics Japan, 1988, 12(5):354～359
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[26] Clements J S, Combined Removal of SO_2/NO_x and Fly Ash from Simulated Flue Gas Using Pulse Streamer Corona, IEEE Trans Ind Appl, 1989, 25(1): 62～69
[27] Dinelli G, Industrial Experiments in Pulse Corona Simultaneous Removal of NOx and SO_2 from Flue Gas, IEEE Trans Ind Appl, 1990, 26(3): 535～541
[28] Giorgio Dinelli, Luigi Civitano, Massimo Rea, Industrial Experiments on Pulse Corona Simultaneous Removal of NO_x and SO_2 from Flus Gas, IEEE Transaction on Industry Application, 1990, May/June, vol. 26, No. 3: 535～541
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