NTP技术转化柴油机NO_x及再生DPF的实验研究和机理分析
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摘要
汽车工业的发展在推动经济与社会发展的同时，不可避免地造成大气污染，严重危及人类健康及生存环境。目前柴油机的NO_x、PM排放后处理技术还不成熟，有必要对其进行改进。本文从实用角度提出了利用低温等离子体技术转化柴油机NO_x及再生微粒捕集器的技术路线，探讨了低温等离子体转化NO_x及再生微粒捕集器的可行性。首先通过静态实验系统研究了介质阻挡放电产生低温等离子体的各主要电学参量的变化规律，并以此为基础设计了适于柴油机后处理的低温等离子体反应器；然后研究了NO／C_3H_6／CO_2/O_2／N_2气氛在低温等离子体反应器中的变化规律，并试图揭示其化学反应机理；最后搭建柴油机台架实验系统，将低温等离子体反应器产生的活性物质喷入到柴油机排气系统中，研究活性物质对柴油机各排放物的处理效果及能力，并研究其对柴油机微粒捕集器的再生能力。本文在以下几方面开展了系统的研究工作：
(1)依据介质阻挡放电理论，进行了静态实验，利用Q-V LissajOUS图形法系统研究了介质厚度、放电气隙、放电频率、激励峰值电压对介质阻挡放电功率、等效电容、电荷传输量、电场强度等表征参数的影响，为研制适于柴油机后处理的低温等离子体反应器提供设计依据。实验结果表明：采用较薄的放电介质以及提高激励峰值电压均可有效提高放电功率、增大电场强度；增大放电频率也可提高放电功率，但其对电场强度的影响不大。
(2)在静态实验研究工作基础上，综合考虑所设计的低温等离子体反应器应满足工作持续时间长、气体过流量大等条件，最后确定同轴单介质低温等离子体反应器的关键结构参数为：石英介质厚度为3mm、放电气隙为2mm，并对其进行了12小时耐久实验测试，实验结果表明，该反应器持续工作时性能稳定、运行可靠。
(3)通过搭建模拟气实验系统，详细研究了低温等离子体对O_2／N_2、NO／O_2／N_2、NO／C_3H_6/O_2／N_2以及NO／N_2、NO／C_3H_6／N_2气氛中NO的转化效率及影响因素，并试图揭示其化学反应机理。实验结果表明：低温等离子体反应器产生的活性物质作用于O_2／N_2气氛时，会产生O_3及NO_2物质；活性物质作用于NO／O_2/N_2气氛时，NO主要通过氧化反应转化为NO_2，降低O_2及NO初始浓度，可提高NO转化率；活性物质作用于NO／C_3H_6/O_2／N_2气氛时，NO同时存在氧化和还原两种途径，C_3H_6初始浓度越高，NO通过还原反应转化为N_2的趋势越明显，同时有CO产生；活性物质作用于NO/N_2气氛时，NO只发生还原反应，转化率低、能耗高，当在其中加入C_3H_6后，可有效提高NO还原效率，并有CO生成。
(4)通过低温等离子体喷射系统处理柴油机模拟排气实验，系统研究了模拟排气温度不同时，低温等离子体反应器产生的活性物质对各模拟排气成分的转化效果。在温度较低时，活性物质主要用于氧化NO为NO_2，NO_x浓度随激励峰值电压的提高基本保持不变；随着温度的升高，活性物质将同时与NO和C_3H_6反应，将NO氧化为NO_2，与C_3H_6反应生成CO：当温度继续升高时，活性物质主要与C_3H_6之间发生氧化反应，生成大量的CO，活性物质对NO的作用相对减弱，故NO转化率降低。
(5)通过将低温等离子体反应器产生的活性物质喷射到柴油机排气系统中，研究柴油机不同工况下活性物质对各排气组分的转化效果及其对微粒捕集器的再生效果。结果表明：柴油机排气温度对转化效果的影响较大，排气温度较低时，活性物质对NO的氧化作用加强，排气中有更多的NO_2生成；排气温度较高时，活性物质同时作用于排气中的NO_X、HC、PM，此时NO转化为NO_2的反应不再明显，另外，由于活性物质对PM作用时会将其表面的有机可溶性成分转化为气态HC物质，故HC浓度略有升高；排气温度更高时，活性物质主要用于分解柴油机排气中的HC及PM，此时CO排放量升高、HC浓度降低。
(6)利用活性炭吸附管对柴油机台架实验两排气支路中微粒捕集器后端的微粒进行吸附，并进行索氏萃取，再利用GC-MS对微粒中的有机可溶性成分进行对比分析。结果表明：低温等离子体反应器产生的活性物质对微粒捕集器确有再生作用，当柴油机在高速大、中负荷工况下运转时，低温等离子体活性物质可以将构成有机可溶性成分的大分子HC物质进行分解或转化，使其部分从微粒表面脱离而转化为气态HC，从而达到再生微粒捕集器的目的；当柴油机在低负荷工况下运转时，由于排气温度较低，活性物质对微粒中有机可溶性成分的分解作用变弱。
Though automobile industry promoted the economic development and social progress, it inevitably brought atmospheric pollution and led to human living environment and health endangered. At the present, the aftetreatrment techniques for controlling NO_x and PM emissions of diesel engine are not yet sophisticated, and need to be improved. In this text, the author presents a technology route using non-thermal plasma to convert NO_x and regenerate diesel paniculate filter from a practical point of view and discusses its feasibility. Firstly of all, main electrical parameters of dielectric barrier discharge have been studied using static experimental system. On this basis, a non-thermal plasma reactor is designed which is suitable for controlling the diesel engine emissions. Secondly, the author studies the changing of NO/C_3H_6/CO_2/O_2/N_2 mixture in the non-thermal plasma reactor and attempts to reveal the chemical reaction mechanisms. Lastly, through building diesel engine bench system, the active substances produced by the non-thermal plasma reactor are injected into the exhaust pipe and its effects for dealing with diesel engine emissions and capacity for regenerating diesel particulate filter are studied. Some researches are made in the text:
(1)Based on dielectric barrier discharge theory, a static experiment system is built to research dielectric barrier discharge characteristics, the effect of dielectric thickness, discharge gap, discharge frequency, excitation peak voltage on the working parameters, such as the power, equivalent capacitance, charge transfer value and electric field intensity, are studied using Q-V Lissajous figures. The experimental results show that: adopting thinner dielectric discharge and smaller discharge gap can improve the discharge power and electric field strength, increasing the discharge frequency may also improve discharge power, but its impact on the electric field strength is little.
(2)On the basis of the results of static experiments and considering that the non-thermal plasma reactor should meet the long work-time and large gas flow conditions, the key structural parameters are finally determined as follows: quartz thickness is 3mm, discharge gap is 2mm. Its 12-hour endurance test result shows that the reactor can stably run for long work-hours.
(3)Through building a simulation gases system, NO conversion efficiency and its influencing factors are studied in detail when O_2/N2, NO/O_2/N_2, NO/C_3H_6/O_2/N_2 and NO/N_2, NO/C_3H_6/N_2 mixture passing the discharge area of the reactor, and the author also attempts to reveal these chemical reaction mechanisms. The experimental results show that: O_3 and NO_2 are produced when the O_2/N_2 mixture passing the discharge area of the non-thermal plasma reactor; when active substances produced by the reactor acting on the NO/O_2/N_2 mixture, NO is mainly oxidized into NO2, and the decrease of O_2 and NO initial concentration can enhance NO conversion rate; In the NO/C_3H_6/O_2/N_2 mixture, NO oxidation and reduction reactions simultaneously exist, the higher C_3H_6 initial concentration is, the easier NO reverts into N_2 through the reduction reaction, at the same time, CO is produced; when the NO/N_2 mixture passing the discharge area of the non-thermal plasma reactor, NO reduction reaction only occurs ,its conversion rate is low and its energy consumption is high, after adding C_3H_6 in the NO/N_2 mixture, NO reduction efficiency can be effectively improved, and CO is also produced.
(4)Through building a non-thermal plasma injection system to deal with diesel engine simulation exhaust, the transformation of simulation exhaust components is studied at the different gas temperature when active substances produced in non-thermal plasma reactor are injected into the exhaust pipe. At the lower temperature, the active substance produced by the reactor mainly oxidize NO into NO_2, the NO_x concentration is almost changeless when excitation peak voltage increases; when the temperature increases, the active substance produced by the reactor simultaneously reacts with NO and C_3H_6, NO is converted to NO2, CO is produced because C_3H_6 is oxidized by the active substance; When the temperature continues to rise, the oxidation reaction between the active substance and C_3H_6 plays a major role, and generate a large number of CO, active substance which oxidize NO becomes less, so the NO conversion rate drops.(5)Through injecting active substance produced by the non-thermal plasma reactor into the diesel exhaust pipe, the transformation effect of exhaust componentsand regeneration efficiency of diesel particulate filter are studied under the diesel different operating conditions. The results showed that: diesel exhaust temperature have a significant impact on the transformation efficiency. When exhaust temperature is low, NO oxidation reaction with the active substances will be strengthened, more NO_2 is generated; when exhaust temperature is high, the active substances simultaneously act on NO_x、HC、PM in the emission pipe, at this time, NO oxidation reaction is not obvious. In addition, HC concentration will slightly increases because active substances will oxidize soluble organic fraction into gaseous HC; when exhaust temperature is more higher, the active substance are mainly used for the decomposition of HC and PM, so CO concentration increased and HC concentration decreased.
(6) In the Bench test, particulate matter after diesel particulate filter which are fixed in diesel engine exhaust pipe are adsorbed using activated carbon adsorption tube. After Soxhlet extraction, the SOF is analyzed by the use of GC-MS. The results show that: the active substance produced by the non-thermal plasma reactor can strictly regenerate diesel particulate filter. When the diesel engine runs at high speed, big or medium load operating conditions, HC macromolecules in the SOF can be decomposed or transformed by the active composition produced by the reactor and are divorced from particulate matter surface, consequently, diesel particulate filter is regenerated; when the diesel engine runs at low load conditions, the decomposition of SOF by active material becomes weaker due to the low exhaust gas temperature.
(1)依据介质阻挡放电理论，进行了静态实验，利用Q-V LissajOUS图形法系统研究了介质厚度、放电气隙、放电频率、激励峰值电压对介质阻挡放电功率、等效电容、电荷传输量、电场强度等表征参数的影响，为研制适于柴油机后处理的低温等离子体反应器提供设计依据。实验结果表明：采用较薄的放电介质以及提高激励峰值电压均可有效提高放电功率、增大电场强度；增大放电频率也可提高放电功率，但其对电场强度的影响不大。
(2)在静态实验研究工作基础上，综合考虑所设计的低温等离子体反应器应满足工作持续时间长、气体过流量大等条件，最后确定同轴单介质低温等离子体反应器的关键结构参数为：石英介质厚度为3mm、放电气隙为2mm，并对其进行了12小时耐久实验测试，实验结果表明，该反应器持续工作时性能稳定、运行可靠。
(3)通过搭建模拟气实验系统，详细研究了低温等离子体对O_2／N_2、NO／O_2／N_2、NO／C_3H_6/O_2／N_2以及NO／N_2、NO／C_3H_6／N_2气氛中NO的转化效率及影响因素，并试图揭示其化学反应机理。实验结果表明：低温等离子体反应器产生的活性物质作用于O_2／N_2气氛时，会产生O_3及NO_2物质；活性物质作用于NO／O_2/N_2气氛时，NO主要通过氧化反应转化为NO_2，降低O_2及NO初始浓度，可提高NO转化率；活性物质作用于NO／C_3H_6/O_2／N_2气氛时，NO同时存在氧化和还原两种途径，C_3H_6初始浓度越高，NO通过还原反应转化为N_2的趋势越明显，同时有CO产生；活性物质作用于NO/N_2气氛时，NO只发生还原反应，转化率低、能耗高，当在其中加入C_3H_6后，可有效提高NO还原效率，并有CO生成。
(4)通过低温等离子体喷射系统处理柴油机模拟排气实验，系统研究了模拟排气温度不同时，低温等离子体反应器产生的活性物质对各模拟排气成分的转化效果。在温度较低时，活性物质主要用于氧化NO为NO_2，NO_x浓度随激励峰值电压的提高基本保持不变；随着温度的升高，活性物质将同时与NO和C_3H_6反应，将NO氧化为NO_2，与C_3H_6反应生成CO：当温度继续升高时，活性物质主要与C_3H_6之间发生氧化反应，生成大量的CO，活性物质对NO的作用相对减弱，故NO转化率降低。
(5)通过将低温等离子体反应器产生的活性物质喷射到柴油机排气系统中，研究柴油机不同工况下活性物质对各排气组分的转化效果及其对微粒捕集器的再生效果。结果表明：柴油机排气温度对转化效果的影响较大，排气温度较低时，活性物质对NO的氧化作用加强，排气中有更多的NO_2生成；排气温度较高时，活性物质同时作用于排气中的NO_X、HC、PM，此时NO转化为NO_2的反应不再明显，另外，由于活性物质对PM作用时会将其表面的有机可溶性成分转化为气态HC物质，故HC浓度略有升高；排气温度更高时，活性物质主要用于分解柴油机排气中的HC及PM，此时CO排放量升高、HC浓度降低。
(6)利用活性炭吸附管对柴油机台架实验两排气支路中微粒捕集器后端的微粒进行吸附，并进行索氏萃取，再利用GC-MS对微粒中的有机可溶性成分进行对比分析。结果表明：低温等离子体反应器产生的活性物质对微粒捕集器确有再生作用，当柴油机在高速大、中负荷工况下运转时，低温等离子体活性物质可以将构成有机可溶性成分的大分子HC物质进行分解或转化，使其部分从微粒表面脱离而转化为气态HC，从而达到再生微粒捕集器的目的；当柴油机在低负荷工况下运转时，由于排气温度较低，活性物质对微粒中有机可溶性成分的分解作用变弱。
Though automobile industry promoted the economic development and social progress, it inevitably brought atmospheric pollution and led to human living environment and health endangered. At the present, the aftetreatrment techniques for controlling NO_x and PM emissions of diesel engine are not yet sophisticated, and need to be improved. In this text, the author presents a technology route using non-thermal plasma to convert NO_x and regenerate diesel paniculate filter from a practical point of view and discusses its feasibility. Firstly of all, main electrical parameters of dielectric barrier discharge have been studied using static experimental system. On this basis, a non-thermal plasma reactor is designed which is suitable for controlling the diesel engine emissions. Secondly, the author studies the changing of NO/C_3H_6/CO_2/O_2/N_2 mixture in the non-thermal plasma reactor and attempts to reveal the chemical reaction mechanisms. Lastly, through building diesel engine bench system, the active substances produced by the non-thermal plasma reactor are injected into the exhaust pipe and its effects for dealing with diesel engine emissions and capacity for regenerating diesel particulate filter are studied. Some researches are made in the text:
(1)Based on dielectric barrier discharge theory, a static experiment system is built to research dielectric barrier discharge characteristics, the effect of dielectric thickness, discharge gap, discharge frequency, excitation peak voltage on the working parameters, such as the power, equivalent capacitance, charge transfer value and electric field intensity, are studied using Q-V Lissajous figures. The experimental results show that: adopting thinner dielectric discharge and smaller discharge gap can improve the discharge power and electric field strength, increasing the discharge frequency may also improve discharge power, but its impact on the electric field strength is little.
(2)On the basis of the results of static experiments and considering that the non-thermal plasma reactor should meet the long work-time and large gas flow conditions, the key structural parameters are finally determined as follows: quartz thickness is 3mm, discharge gap is 2mm. Its 12-hour endurance test result shows that the reactor can stably run for long work-hours.
(3)Through building a simulation gases system, NO conversion efficiency and its influencing factors are studied in detail when O_2/N2, NO/O_2/N_2, NO/C_3H_6/O_2/N_2 and NO/N_2, NO/C_3H_6/N_2 mixture passing the discharge area of the reactor, and the author also attempts to reveal these chemical reaction mechanisms. The experimental results show that: O_3 and NO_2 are produced when the O_2/N_2 mixture passing the discharge area of the non-thermal plasma reactor; when active substances produced by the reactor acting on the NO/O_2/N_2 mixture, NO is mainly oxidized into NO2, and the decrease of O_2 and NO initial concentration can enhance NO conversion rate; In the NO/C_3H_6/O_2/N_2 mixture, NO oxidation and reduction reactions simultaneously exist, the higher C_3H_6 initial concentration is, the easier NO reverts into N_2 through the reduction reaction, at the same time, CO is produced; when the NO/N_2 mixture passing the discharge area of the non-thermal plasma reactor, NO reduction reaction only occurs ,its conversion rate is low and its energy consumption is high, after adding C_3H_6 in the NO/N_2 mixture, NO reduction efficiency can be effectively improved, and CO is also produced.
(4)Through building a non-thermal plasma injection system to deal with diesel engine simulation exhaust, the transformation of simulation exhaust components is studied at the different gas temperature when active substances produced in non-thermal plasma reactor are injected into the exhaust pipe. At the lower temperature, the active substance produced by the reactor mainly oxidize NO into NO_2, the NO_x concentration is almost changeless when excitation peak voltage increases; when the temperature increases, the active substance produced by the reactor simultaneously reacts with NO and C_3H_6, NO is converted to NO2, CO is produced because C_3H_6 is oxidized by the active substance; When the temperature continues to rise, the oxidation reaction between the active substance and C_3H_6 plays a major role, and generate a large number of CO, active substance which oxidize NO becomes less, so the NO conversion rate drops.(5)Through injecting active substance produced by the non-thermal plasma reactor into the diesel exhaust pipe, the transformation effect of exhaust componentsand regeneration efficiency of diesel particulate filter are studied under the diesel different operating conditions. The results showed that: diesel exhaust temperature have a significant impact on the transformation efficiency. When exhaust temperature is low, NO oxidation reaction with the active substances will be strengthened, more NO_2 is generated; when exhaust temperature is high, the active substances simultaneously act on NO_x、HC、PM in the emission pipe, at this time, NO oxidation reaction is not obvious. In addition, HC concentration will slightly increases because active substances will oxidize soluble organic fraction into gaseous HC; when exhaust temperature is more higher, the active substance are mainly used for the decomposition of HC and PM, so CO concentration increased and HC concentration decreased.
(6) In the Bench test, particulate matter after diesel particulate filter which are fixed in diesel engine exhaust pipe are adsorbed using activated carbon adsorption tube. After Soxhlet extraction, the SOF is analyzed by the use of GC-MS. The results show that: the active substance produced by the non-thermal plasma reactor can strictly regenerate diesel particulate filter. When the diesel engine runs at high speed, big or medium load operating conditions, HC macromolecules in the SOF can be decomposed or transformed by the active composition produced by the reactor and are divorced from particulate matter surface, consequently, diesel particulate filter is regenerated; when the diesel engine runs at low load conditions, the decomposition of SOF by active material becomes weaker due to the low exhaust gas temperature.
引文
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