脉冲放电脱硫反应器电参数测量及结构优化
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摘要
本课题运用实验方法对脉冲放电低温等离子体线—板式脱硫反应器的放电特性、电极配置形式对脱硫效率的影响以及脉冲能量沿放电线的传输进行了较为深入和系统的研究，目的是为该技术的工业化应用提供科学依据。主要研究内容和结论有：
1、在室温、空气介质条件下，研究了不同初级电压、不同成形电容匹配、不同线板间距、不同放电极邻距等因素对放电特性的影响，得到了反应器的放电规律：脉冲峰值电压、基压和拖尾电压随放电极邻距的增大先减小，然后增大；脉冲能量则随放电极邻距的增大先增大，然后减小。并根据本实验结果，得出了反应器线—板结构优化配置的经验公式b=0.3c+3.75(式中b为放电线间距，c为线—板间距，单位都是cm)。
2、经过对放电极在不同脉冲峰值电压、不同末端匹配、不同放电线直径下进行的能量衰减实验研究，得到了高压脉冲能量在电晕放电极上以行波形式传播、衰减的规律：高压脉冲能量沿电晕线迅速衰减，脉冲波形显著畸变；峰值电压越高，电晕线越细，放电越强，衰减越快；电晕线尾端受行波反射影响较大。并得出：在进行反应器的设计时，为提高脱硫效率和能量利用率，合理设计反应器的尺寸，提高反应器的性价比，放电线的长度不宜过长，一般不应超过10m。
3、在烟气量为200Nm~3/h烟气脱硫装置上进行了脱硫实验研究，通过脱硫率与电极结构和电源匹配关系的研究结果，验证了反应器结构优化的经验公式，并提高了脱硫效率。
In this paper, detailed studies were made on discharge characteristics of pulse corona reactor, the influences of electrode configuration on desulfurization and pulse energy transmission along the discharge wires for industrial application of the technique. The following results were obtained.
1. The influence factors (such as voltage, pulse forming capacitance, wire-to-plate spacing, wire-to-wire spacing) on discharge characteristics are researched on the condition of room temperature and air medium, and the discharge characteristics of reactor are obtained: the peak value, minimum value and wave tail of pulse voltage firstly increase with the increase of wire-to-wire spacing, then all decrease; but pulse energy firstly decreases with the increase of wire-to-wire spacing, then increases. According to experimental conclusion, the experimental formula of the optimized electrode configuration, b=0.3c+37.5 (b, wire-to-wire spacing; c, wire-to-plate spacing) is gotten.
2. The attenuation and distortion law of pulse voltage transmitting on discharge electrode is obtained by research of energy attenuation on different conditions (such as voltage, terminal matching and diameter). Pulse voltage sharply decreases due to the corona. The higher the pulse voltage, the thinner the diameter of the wire, then the more seriously the pulse voltage attenuates; the tail of the corona wire is more influenced by the reverberation. The sharp attenuation of the corona along the wire has to be considered in designing a real reactor for getting higher reacting efficiency and the length of wire should be no more than 1 Om.
3. On the basis of above-mentioned experimental conclusions, an experimental desulfurization system with the flux of 200Nm3/h is optimized, and preferable efficiency of desulfurization is obtained.
1、在室温、空气介质条件下，研究了不同初级电压、不同成形电容匹配、不同线板间距、不同放电极邻距等因素对放电特性的影响，得到了反应器的放电规律：脉冲峰值电压、基压和拖尾电压随放电极邻距的增大先减小，然后增大；脉冲能量则随放电极邻距的增大先增大，然后减小。并根据本实验结果，得出了反应器线—板结构优化配置的经验公式b=0.3c+3.75(式中b为放电线间距，c为线—板间距，单位都是cm)。
2、经过对放电极在不同脉冲峰值电压、不同末端匹配、不同放电线直径下进行的能量衰减实验研究，得到了高压脉冲能量在电晕放电极上以行波形式传播、衰减的规律：高压脉冲能量沿电晕线迅速衰减，脉冲波形显著畸变；峰值电压越高，电晕线越细，放电越强，衰减越快；电晕线尾端受行波反射影响较大。并得出：在进行反应器的设计时，为提高脱硫效率和能量利用率，合理设计反应器的尺寸，提高反应器的性价比，放电线的长度不宜过长，一般不应超过10m。
3、在烟气量为200Nm~3/h烟气脱硫装置上进行了脱硫实验研究，通过脱硫率与电极结构和电源匹配关系的研究结果，验证了反应器结构优化的经验公式，并提高了脱硫效率。
In this paper, detailed studies were made on discharge characteristics of pulse corona reactor, the influences of electrode configuration on desulfurization and pulse energy transmission along the discharge wires for industrial application of the technique. The following results were obtained.
1. The influence factors (such as voltage, pulse forming capacitance, wire-to-plate spacing, wire-to-wire spacing) on discharge characteristics are researched on the condition of room temperature and air medium, and the discharge characteristics of reactor are obtained: the peak value, minimum value and wave tail of pulse voltage firstly increase with the increase of wire-to-wire spacing, then all decrease; but pulse energy firstly decreases with the increase of wire-to-wire spacing, then increases. According to experimental conclusion, the experimental formula of the optimized electrode configuration, b=0.3c+37.5 (b, wire-to-wire spacing; c, wire-to-plate spacing) is gotten.
2. The attenuation and distortion law of pulse voltage transmitting on discharge electrode is obtained by research of energy attenuation on different conditions (such as voltage, terminal matching and diameter). Pulse voltage sharply decreases due to the corona. The higher the pulse voltage, the thinner the diameter of the wire, then the more seriously the pulse voltage attenuates; the tail of the corona wire is more influenced by the reverberation. The sharp attenuation of the corona along the wire has to be considered in designing a real reactor for getting higher reacting efficiency and the length of wire should be no more than 1 Om.
3. On the basis of above-mentioned experimental conclusions, an experimental desulfurization system with the flux of 200Nm3/h is optimized, and preferable efficiency of desulfurization is obtained.
引文
[1]郝吉明等．燃煤二氧化硫污染控制技术手册．北京：化学工业出版社，2001，2-3
[2]国家环境保护总局．2001年中国环境状况公报
[3]郝吉明等．燃煤二氧化硫污染控制技术手册．北京：化学工业出版社，2001，7-9
[4]国家环境保护“十五”计划
[5]Masuada S. "Pulse corona induced plasma chemical process: a horizon of new plasma chemical technologies"[J]. Pure Appl.Chen. 1998, 6:727
[6]Masuada S., Wu Yan, et al. Pulse corona induced plasma chemical process for De-NO_x, De-SO_2, and mercury vapor control of combustion gas. Third Int. Conf. Electrostatic Precipitation, M.Rea.ED. 1987,pp667-676
[7]Masuada S., Wu Yan, et al. DeNOx and control of mercury vapor from combustion gas by pulse corona induced plasma chemical process (PPCP), ISPC-8, Tokyo, 1987,pp. 2222-2227
[8]Dinelli G, Civitano L., and Rea M., Industrial experiments on pulse simultaneous removal of NO_x and SO_2, from flue gas. IEEE Trans. Ind.Appl.25, 1990,535-541
[9]Denial G, Civitano L., and Rea M., Industrial experiments on pulse simultaneous removal of NO_x and SO_2, from flue gas by means of impulse streamer corona. Trans IEEE-IAS 25,1989,62-69
[10]Y.H Song et al.,"A Industrial-Scale Experiment of Pulse Corona process for Removing NO_x and SO_2 from Combustion flue gas"[J] J.Adv. Oxid. Techlo. 1997, 2(2) 268
[11]吴彦，张彦彬，朱益民．脉冲放电脱硫技术的小试研究．中国物理学会第七界静电学术年会论文集：经典基础及应用技术，1996，50-53
[12]Wu Y., et al. Industrial Experiments on generator and reactor system for SO_2 removal from flue gas by pulse corona discharge, Proc.3rd Int. Conf. Appl. Electrostatics, Shanghai, pp. 8-11
[13]张彦彬，王宁会，吴彦．3000Nm~3/h烟气脱硫实验系统的设计与运行．大连理工大学学报Vol．37，No．5，1997，551-554
[14]赵志斌，吴彦，王宁会．含水烟气脉冲放电脱硫脱硝的研究．大连理工大学学报．Vol．6，No．4，1996，424-429
[15]Wu yan, Zhu yimin, Wang Ninghui. Investigation no SO_2 and NO_x removal from flue gas by pulsed corona discharge. Proceeding, ICESP Ⅶ Sep.20-25, 1998,Kyongju, Korea, pp.212-215
[16]Massimo Reaetal. Energization of pulse corona induced chemical process, Non-Thermal Plasma Techniques for Pollution Control, G34(A), 1993:191-204
[17]YanKeping etal. Matching between voltage pulse generator and reactor for producing low temperature plasma by positive pulse corona, 2nd Int. Conf. Applied Electrostatics, Beijing, 1993,pp.83-95
[18]M.Laan. et al.,"The Multi-avalanche nature of streamer for mation in inhomogeneous fields"[J]. J.Phys.D: Appl.Phys. 1994(27)970.
[19]I.Gallimberti "Impulse corona simulation for flue gas treatment"[J]. Pure Appl.Chem.5(1988)Norman.
[20]Busi F., et al., Radiation induced NO_x/SO_2 emission control for industrial and power plant flue gas, Radiat. Phys. Chem. 1985, 31:101-108
[21]Busi F., et al., A kinetic model for radiation treatment of combustion gas, Science of the total environment,
64,1987:pp.233-238
[22]Tokunaga O. and N.Suzuki, Radiation chemical reaction in SO_2 and NO_x removal from flue gas, Radiat, Phys. Chem. 1984, 24:145-165
[23]Clavert J.G, et al., Chemical mechanisms of acid generation in the troposphere, Nature 1985,317,pp,27-35
[24]Matzing H., Chemical kinetics of flue gas cleaning by irradiation with electron, Advance in Chemical Physics Volume LXXX, ed.by I. Prigogine and Stuart A.Rice, Jone Wiley and Sons Inc., 1991,pp.315-401
[25]Chang J. S., and Masuda M., Mechanism of pulse corona induced plasma chemical process for removal of NOx and SO_2 from combustion flue gas, in IEEE Ind. Appl. Soc. 1998 Meeting, pp.1645-1653
[26]Mizuno A., Clements J. S. and R. H. Davis, Combined treatment of SO_2 and high resistively fly ash using a pulse energized electron reactor, Proc. Ind. Int. Conf., Electrostatic precipitation, Tokyo, Japan, 1984, pp.879-885
[27]Civitano L., et al., DeNO_x and DeSO_x process by gas energisation, in: Plasma Technology: fundamentals and applications, ed. by Capitelli M., Gorse C., Plenum press, 1992,pp.153-166
[28]李杰等．脉冲放电等离子体烟气脱硫中水蒸气活化作用．大连理工大学学报．Vol．40，No．3，May．2000，pp．267-269
[29]Masuda S. et al., A pulse voltage sources for electrostatic precipitators, IEEE Ind. Appl. Soc. Annu. Meeting, Toronto, ON Canada, 1978
[30]吴彦等．电晕法脱硫脱硝电源/反应器研究．大连理工大学学报．Vol．35，No．1，Feb．1995，pp．31-34
[31]赵君科等．脉冲电云等离子体法烟气脱硫脱硝进展．四川环境2000年第19卷第4起，6-8
[32]Youhei Kinoshita, Keita Saito, Kazunori Takashima, Shinji Katsura, and Akira Mizuno,"Removal of SO2 Using a Wet-Type Non-Thermal Plasma Reactor",IEEE Trans. Ind. Appl., 2001,693—697
[33]Isao Yamamoto, Kochi Yamamoto, Kotaro Shimizu, Yuichi Fujiyama, Kazuhiko Tsunoda and Akira Mizuno, "Wet type plasma reactor for incinerator", IEEE Trans. Ind. Appl., 1998,1861—1864
[34]Atkinson, R.,"Kinetics and mechanisms of the gas-phase reactions of the hydroxyl radical with organic compounds under atmospheric conditions" Chem. Re. 1985,85:69—201
[35]Shunsuke Hosokawa ,"Application of PPCP for reduction gaseous pollutants exhausted from encineration plant", Proc. of NEDO Symp. on Non-thermal Discharge Plasma Technology for Air Pollution Control, 1997,109—114
[36]T. Ohkubo, S, Kanazawa, Y.Nomoto and J.S.Chang, "Corona induced non-thermal plasma for NO_x removal: packed-bed reactor and streamer corona radical shower system", Proc. of NEDO Symp. on Non-thermal Discharge Plasma Technology for Air Pollution Control, 1997, 11—12
[37]Toshiaki Yamamoto, "Soft plasma for HAP decomposition", Proc. Of NEDO Symp. on Non-thermal Discharge Plasma Technology for Air Pollution Control, 1997,38—48
[38]Zhenzhou SU, Yoshihiko Matsui, Kazunori Takashima, Shinji Katsura and Akira Mizuno, "The Combination of Non-thermal Plasma and BaO catalyst for NO_x Storage-Reduction Process", The 4th int. Conf. Appl. Eleclrostatics, 2001,278—281
[39]Ohkubo T, Kanazawa S, Nomoto Y, et al. "NO_x removal by a pipe with nozzle-plate electrode corona discharge system[J]" J.Electrostatics, 1990,25:23-40.
[40]李杰，吴彦，王宁会，张彦彬．脉冲放电等离子体烟气脱硫中水蒸气活化作用．大连理工大学学报，Vol．40，No．3，May 2000，267—269
[41]Jae-Duk Moon, Geun-Taek Lee, and Suk-Hwan Chung, "SO and CO Gas Removal and Discharge
Characteristics of a Nonthermal Plasma Reactor in a Crossed DC Magnetic Field", IEEE Trans. Ind. Appl., 1990,35:1198-1204
[42]李国锋等．脉冲电晕脱硫脱硝反应器电极配置研究．大连理工大学学报．Vol．39，No．1，Jan 1999，39-42
[43]李国锋，吴彦，王宁会．线—板式脉冲电晕放电系统研究．高电压技术．Vol．25，No．1，Jan 1999，4-6
[44]李国锋，吴彦，王宁会．脉冲电晕放电特性研究．大连理工大学学报．Vol．139，No．6，Nov 1999，736-740
[45]李国锋，吴彦．脉冲放电等离子体化学(PPCP)处理有害气体反应器的研究进展．环境科学进展．Vol．7，No．4，Aug 1999，54-59
[46]李国锋，唐本峰，吴彦．脉冲电晕放电过程中火花放电的研究．中国物理学会第8届静电学术年会会议文集：现代静电科学技术研究，Aug 1999，58-60
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[50]S. Masuda, K. Akutsu, M. Kuroda. A ceramic-based ozonizer using high frequency discharge. Proc. IEEE/IAS Annual Conf. Tronto Canada. 1985, 1353-1358
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[52]S.Masuda and H.Nakao. Control of NO_x by positive and negative pulsed corona discharges. Proc. IEEE/IAS Ann, Meeting, USA Denver: 1986, 1173-1182
[2]国家环境保护总局．2001年中国环境状况公报
[3]郝吉明等．燃煤二氧化硫污染控制技术手册．北京：化学工业出版社，2001，7-9
[4]国家环境保护“十五”计划
[5]Masuada S. "Pulse corona induced plasma chemical process: a horizon of new plasma chemical technologies"[J]. Pure Appl.Chen. 1998, 6:727
[6]Masuada S., Wu Yan, et al. Pulse corona induced plasma chemical process for De-NO_x, De-SO_2, and mercury vapor control of combustion gas. Third Int. Conf. Electrostatic Precipitation, M.Rea.ED. 1987,pp667-676
[7]Masuada S., Wu Yan, et al. DeNOx and control of mercury vapor from combustion gas by pulse corona induced plasma chemical process (PPCP), ISPC-8, Tokyo, 1987,pp. 2222-2227
[8]Dinelli G, Civitano L., and Rea M., Industrial experiments on pulse simultaneous removal of NO_x and SO_2, from flue gas. IEEE Trans. Ind.Appl.25, 1990,535-541
[9]Denial G, Civitano L., and Rea M., Industrial experiments on pulse simultaneous removal of NO_x and SO_2, from flue gas by means of impulse streamer corona. Trans IEEE-IAS 25,1989,62-69
[10]Y.H Song et al.,"A Industrial-Scale Experiment of Pulse Corona process for Removing NO_x and SO_2 from Combustion flue gas"[J] J.Adv. Oxid. Techlo. 1997, 2(2) 268
[11]吴彦，张彦彬，朱益民．脉冲放电脱硫技术的小试研究．中国物理学会第七界静电学术年会论文集：经典基础及应用技术，1996，50-53
[12]Wu Y., et al. Industrial Experiments on generator and reactor system for SO_2 removal from flue gas by pulse corona discharge, Proc.3rd Int. Conf. Appl. Electrostatics, Shanghai, pp. 8-11
[13]张彦彬，王宁会，吴彦．3000Nm~3/h烟气脱硫实验系统的设计与运行．大连理工大学学报Vol．37，No．5，1997，551-554
[14]赵志斌，吴彦，王宁会．含水烟气脉冲放电脱硫脱硝的研究．大连理工大学学报．Vol．6，No．4，1996，424-429
[15]Wu yan, Zhu yimin, Wang Ninghui. Investigation no SO_2 and NO_x removal from flue gas by pulsed corona discharge. Proceeding, ICESP Ⅶ Sep.20-25, 1998,Kyongju, Korea, pp.212-215
[16]Massimo Reaetal. Energization of pulse corona induced chemical process, Non-Thermal Plasma Techniques for Pollution Control, G34(A), 1993:191-204
[17]YanKeping etal. Matching between voltage pulse generator and reactor for producing low temperature plasma by positive pulse corona, 2nd Int. Conf. Applied Electrostatics, Beijing, 1993,pp.83-95
[18]M.Laan. et al.,"The Multi-avalanche nature of streamer for mation in inhomogeneous fields"[J]. J.Phys.D: Appl.Phys. 1994(27)970.
[19]I.Gallimberti "Impulse corona simulation for flue gas treatment"[J]. Pure Appl.Chem.5(1988)Norman.
[20]Busi F., et al., Radiation induced NO_x/SO_2 emission control for industrial and power plant flue gas, Radiat. Phys. Chem. 1985, 31:101-108
[21]Busi F., et al., A kinetic model for radiation treatment of combustion gas, Science of the total environment,
64,1987:pp.233-238
[22]Tokunaga O. and N.Suzuki, Radiation chemical reaction in SO_2 and NO_x removal from flue gas, Radiat, Phys. Chem. 1984, 24:145-165
[23]Clavert J.G, et al., Chemical mechanisms of acid generation in the troposphere, Nature 1985,317,pp,27-35
[24]Matzing H., Chemical kinetics of flue gas cleaning by irradiation with electron, Advance in Chemical Physics Volume LXXX, ed.by I. Prigogine and Stuart A.Rice, Jone Wiley and Sons Inc., 1991,pp.315-401
[25]Chang J. S., and Masuda M., Mechanism of pulse corona induced plasma chemical process for removal of NOx and SO_2 from combustion flue gas, in IEEE Ind. Appl. Soc. 1998 Meeting, pp.1645-1653
[26]Mizuno A., Clements J. S. and R. H. Davis, Combined treatment of SO_2 and high resistively fly ash using a pulse energized electron reactor, Proc. Ind. Int. Conf., Electrostatic precipitation, Tokyo, Japan, 1984, pp.879-885
[27]Civitano L., et al., DeNO_x and DeSO_x process by gas energisation, in: Plasma Technology: fundamentals and applications, ed. by Capitelli M., Gorse C., Plenum press, 1992,pp.153-166
[28]李杰等．脉冲放电等离子体烟气脱硫中水蒸气活化作用．大连理工大学学报．Vol．40，No．3，May．2000，pp．267-269
[29]Masuda S. et al., A pulse voltage sources for electrostatic precipitators, IEEE Ind. Appl. Soc. Annu. Meeting, Toronto, ON Canada, 1978
[30]吴彦等．电晕法脱硫脱硝电源/反应器研究．大连理工大学学报．Vol．35，No．1，Feb．1995，pp．31-34
[31]赵君科等．脉冲电云等离子体法烟气脱硫脱硝进展．四川环境2000年第19卷第4起，6-8
[32]Youhei Kinoshita, Keita Saito, Kazunori Takashima, Shinji Katsura, and Akira Mizuno,"Removal of SO2 Using a Wet-Type Non-Thermal Plasma Reactor",IEEE Trans. Ind. Appl., 2001,693—697
[33]Isao Yamamoto, Kochi Yamamoto, Kotaro Shimizu, Yuichi Fujiyama, Kazuhiko Tsunoda and Akira Mizuno, "Wet type plasma reactor for incinerator", IEEE Trans. Ind. Appl., 1998,1861—1864
[34]Atkinson, R.,"Kinetics and mechanisms of the gas-phase reactions of the hydroxyl radical with organic compounds under atmospheric conditions" Chem. Re. 1985,85:69—201
[35]Shunsuke Hosokawa ,"Application of PPCP for reduction gaseous pollutants exhausted from encineration plant", Proc. of NEDO Symp. on Non-thermal Discharge Plasma Technology for Air Pollution Control, 1997,109—114
[36]T. Ohkubo, S, Kanazawa, Y.Nomoto and J.S.Chang, "Corona induced non-thermal plasma for NO_x removal: packed-bed reactor and streamer corona radical shower system", Proc. of NEDO Symp. on Non-thermal Discharge Plasma Technology for Air Pollution Control, 1997, 11—12
[37]Toshiaki Yamamoto, "Soft plasma for HAP decomposition", Proc. Of NEDO Symp. on Non-thermal Discharge Plasma Technology for Air Pollution Control, 1997,38—48
[38]Zhenzhou SU, Yoshihiko Matsui, Kazunori Takashima, Shinji Katsura and Akira Mizuno, "The Combination of Non-thermal Plasma and BaO catalyst for NO_x Storage-Reduction Process", The 4th int. Conf. Appl. Eleclrostatics, 2001,278—281
[39]Ohkubo T, Kanazawa S, Nomoto Y, et al. "NO_x removal by a pipe with nozzle-plate electrode corona discharge system[J]" J.Electrostatics, 1990,25:23-40.
[40]李杰，吴彦，王宁会，张彦彬．脉冲放电等离子体烟气脱硫中水蒸气活化作用．大连理工大学学报，Vol．40，No．3，May 2000，267—269
[41]Jae-Duk Moon, Geun-Taek Lee, and Suk-Hwan Chung, "SO and CO Gas Removal and Discharge
Characteristics of a Nonthermal Plasma Reactor in a Crossed DC Magnetic Field", IEEE Trans. Ind. Appl., 1990,35:1198-1204
[42]李国锋等．脉冲电晕脱硫脱硝反应器电极配置研究．大连理工大学学报．Vol．39，No．1，Jan 1999，39-42
[43]李国锋，吴彦，王宁会．线—板式脉冲电晕放电系统研究．高电压技术．Vol．25，No．1，Jan 1999，4-6
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