处理低浓度有机废气的流向变换催化燃烧反应技术研究
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摘要
流向变换催化燃烧技术是人为非定态操作的一种,结合蓄热换热器和催化燃烧两种技术的特点,通过周期性地切换固定床催化反应器内的气流方向,使床层内出现中间高、两边低的温度分布,因而适合于进行反应物浓度较低的不可逆强放热反应或放热较弱的可逆反应,能够提高反应效率和对产物的选择性。本文主要围绕将流向变换催化燃烧技术应用于工业过程中低浓度有机废气净化而展开,讨论该类型反应器的基本运行特性、失稳条件以相应的控制措施。
首先,自行设计搭建了小型流向变换催化燃烧反应系统,并在此系统上进行了冷态条件下系统流动阻力特性试验研究。随着流向的周期性切换,床层的压降也随之呈现周期性的变化。在气流流向发生切换后的瞬间,床层内的流动状况需历经一定的波动方能达到稳定,但由于该过渡状态对于反应器整体操作过程影响基本可以忽略。稳定后的床层压降变化规律可以用Ergun方程来描述,即压降随表观气速的增大呈二次曲线的形式上升,随床层高度的增加而呈线性增长。根据试验数据,回归得到用于描述本反应系统压降变化的数学关联式,该关联式可较好地预测床层内的压降变化。
随后,进行了低浓度甲烷和苯的催化燃烧试验研究,讨论了操作条件对反应器运行特性的影响。基本上,随着周期性的流向切换,反应器内各个测点温度也随之作周期性波动变化；只要能够维持反应器自热运行,反应器内整体净化率可达到98%以上,且不存在NOx等的二次污染。提高入口反应物浓度和缩短流向切换周期度,都会使得催化段的温度水平和反应器内最高温度上升,增加中间高温平台的宽度,令燃烧效率提升。表观气速的影响是反应器内反应放热和传热条件综合作用的结果。当甲烷和苯两种性质相差较大的有机物在反应器内协同燃烧净化时,反应器内的温度水平和轴向温度分布会甲烷浓度的随着升高而升高,苯的燃烧净化效率基本保持在95%以上。降低入口反应物浓度、延长流向切换时间可以降低反应器内出现“M”型温度分和发生“飞温”的可能。而采用辅助电加热或者添加辅助燃料的方法都可以有效避免入口浓度过低时反应器出现“熄火”现象。但如果所添加的辅助燃料与待处理有机物的催化燃烧性质差异过大,会显著增加辅助燃料的消耗量。
接着,建立了用于描述该种类型反应器行为的一维瞬态非均相数学模型。模拟计算的结果能较好地反映小型流向变换催化燃烧器的实际运行特性。
基于上述模型,讨论了反应器壁面、床层内传递参数和反应动力学参数对反应器运行特性的影响。在横向比较各种操作参数对反应器运行特性的影响时,提出采用热波移动距离作为衡量的标准。通过在对各种操作参数影响的比较,认为在本文所选用的反应器参数范围内,当表观气速在0.2～0.4m·s-1左右,热波移动距离在约占催化床层长度的20～40%,惰性段装填比例在20～40%之间时,反应器具有较高的热稳定性和较宽的可操作域,并且可适应于更低的入口浓度条件。
然后,通过试验和数值模拟两方面的研究,讨论了当入口条件发生周期性波动时流向变换催化燃烧反应器的运行特性。结果表明,入口浓度的周期性波动会降低反应器内的温度水平,削弱反应器的稳定性,甚至可能导致最终发生熄火。在此情形下,适当调整流向切换周期是维持反应器稳定运行的较好手段。基于上述结果,从动态系统的角度提出了流向变换催化燃烧反应器的特征响应时间的概念,并采用谐波分析的方法对此加以系统阐释,并解释了当入口浓度波动的频率和反应器流向切换频率相同时,反应器最高温度发生大幅度波动的原因。在此基础上,模拟验证了在系统发生谐波响应时,通过改变系统的特征响应时间来维持反应器稳定的可行性。
最后,试验和数值模拟结果,以处理60000m3·h-1有机废气的工程实例为典型,分析了将流向变换催化燃烧技术用于实际工程系统的可行性与经济效益。
Reverse flow reactor (RFR) is an integration of regenerative heat exchanger and fixed bed, in which flow direction is periodically changed. Applying such forced unsteady state operation (FUSO), a hot zone is trapped in the central catalytic section, which suits for exothermal catalytic reaction with low inlet concentration or reversible exothermal reaction with mild reaction heat release. Thus an increase in reactant conversion or product selectivity can be expected. This paper presents experimental and numerical results of the behavior of a bench-scale RFR, which is considered as a proper technology for decontaminating lean volatile organic compounds (VOCs) in waste gas. Effects of operation conditions on reactor behavior and corresponding control strategies when reactor stability is impaired are discussed.
A bench-scale RFR is built up, on which pressure drop through the reactor is studied. The results show that with periodic flow reversal, pressure drop of the reactor changes periodically. It takes several seconds to get a stable flow condition in the reactor soon after the flow reversal. However, effect of such temporary states on reactor behavior is rather since it is very short comparing to flow reversal time. Total pressure drop through the reactor can be calculated by Ergun equation very well, based on regression of experimental data, which means the pressure drop shows a quadratic increase of superficial velocity and a liner increase of bed depth.
Effects of operation parameters on reactor behavior are discussed, taking methane or benzene as model reactant. Temperature in the reactor varies periodically with flow reversal, while conversions of VOCs are all above98%if an auto-thermal operation is maintainded. Little NOx is detected. Basically, increasing inlet combustibles concentration or shortening flow reversal time will result in a higher thermal level and wider temperature plateau in reactor, which increase the VOCs conversion as well. Effect of superficial velocity is co-effect of heat release and convection. When binary mixture of methane and benzene is combusted in RFR, thermal level in reactor increases with the increasing of methane portion. Conversion of benzene is above95%. To eliminate the possibility of reactor thermal run away, decreasing inlet concentration or lengthening flow reversal time are all feasible ways. While using electrical heater or adding auxiliary fuel can increase reactor thermal lever, avoiding reactor extinction. But if methane is added as auxiliary fuel, large amount of methane is needed.
A one-dimensional heterogeneous is built up. Good accordance between simulation and experimental results are acquired.
Effect of reactor wall, transport parameters and reaction kinetics are discussed, based on numerical simulation. Moving range of heat wave is chosen as criterion when comparing effects of various operation parameters on reactor behavior. With parameters applied in this study, following optimum range of operation parameters are proposed, with superficial velocity of0.2～0.4m·s-1, moving range of heat wave taking20～40%of catalytic bed length and a inert packing taking20～40%of total reactor. Within this range, reactor operates more stable and lower minimum inlet concentration is required in maintaining auto-thermal operation.
Effect of periodic inlet concentration is studied. The results show that reactor stability is impaired in such situation, decreasing of reactor thermal level may even cause reactor extinction. Adjusting flow reversal time turns out to be a proper way in maintaining reactor stability. Based on experimental and numerical results, flow reversal time is regarded as characteristic response time of the reaction system. The reason why synchronizing between periodic inlet variation cycle and flow reversal cycle leads to dramatic maximum temperature variation is explained adopting harmonic analysis. According to this theory, the feasibility of changing system characteristic response time in maintaining stable operation is verified by numerical simulation.
With the results acquired in experiments and numerical simulation, a industrial scale reverse flow reactor for purifying waste gas flow of60000m·3h-1is designed, including system feasibility and economical analysis.
首先,自行设计搭建了小型流向变换催化燃烧反应系统,并在此系统上进行了冷态条件下系统流动阻力特性试验研究。随着流向的周期性切换,床层的压降也随之呈现周期性的变化。在气流流向发生切换后的瞬间,床层内的流动状况需历经一定的波动方能达到稳定,但由于该过渡状态对于反应器整体操作过程影响基本可以忽略。稳定后的床层压降变化规律可以用Ergun方程来描述,即压降随表观气速的增大呈二次曲线的形式上升,随床层高度的增加而呈线性增长。根据试验数据,回归得到用于描述本反应系统压降变化的数学关联式,该关联式可较好地预测床层内的压降变化。
随后,进行了低浓度甲烷和苯的催化燃烧试验研究,讨论了操作条件对反应器运行特性的影响。基本上,随着周期性的流向切换,反应器内各个测点温度也随之作周期性波动变化；只要能够维持反应器自热运行,反应器内整体净化率可达到98%以上,且不存在NOx等的二次污染。提高入口反应物浓度和缩短流向切换周期度,都会使得催化段的温度水平和反应器内最高温度上升,增加中间高温平台的宽度,令燃烧效率提升。表观气速的影响是反应器内反应放热和传热条件综合作用的结果。当甲烷和苯两种性质相差较大的有机物在反应器内协同燃烧净化时,反应器内的温度水平和轴向温度分布会甲烷浓度的随着升高而升高,苯的燃烧净化效率基本保持在95%以上。降低入口反应物浓度、延长流向切换时间可以降低反应器内出现“M”型温度分和发生“飞温”的可能。而采用辅助电加热或者添加辅助燃料的方法都可以有效避免入口浓度过低时反应器出现“熄火”现象。但如果所添加的辅助燃料与待处理有机物的催化燃烧性质差异过大,会显著增加辅助燃料的消耗量。
接着,建立了用于描述该种类型反应器行为的一维瞬态非均相数学模型。模拟计算的结果能较好地反映小型流向变换催化燃烧器的实际运行特性。
基于上述模型,讨论了反应器壁面、床层内传递参数和反应动力学参数对反应器运行特性的影响。在横向比较各种操作参数对反应器运行特性的影响时,提出采用热波移动距离作为衡量的标准。通过在对各种操作参数影响的比较,认为在本文所选用的反应器参数范围内,当表观气速在0.2～0.4m·s-1左右,热波移动距离在约占催化床层长度的20～40%,惰性段装填比例在20～40%之间时,反应器具有较高的热稳定性和较宽的可操作域,并且可适应于更低的入口浓度条件。
然后,通过试验和数值模拟两方面的研究,讨论了当入口条件发生周期性波动时流向变换催化燃烧反应器的运行特性。结果表明,入口浓度的周期性波动会降低反应器内的温度水平,削弱反应器的稳定性,甚至可能导致最终发生熄火。在此情形下,适当调整流向切换周期是维持反应器稳定运行的较好手段。基于上述结果,从动态系统的角度提出了流向变换催化燃烧反应器的特征响应时间的概念,并采用谐波分析的方法对此加以系统阐释,并解释了当入口浓度波动的频率和反应器流向切换频率相同时,反应器最高温度发生大幅度波动的原因。在此基础上,模拟验证了在系统发生谐波响应时,通过改变系统的特征响应时间来维持反应器稳定的可行性。
最后,试验和数值模拟结果,以处理60000m3·h-1有机废气的工程实例为典型,分析了将流向变换催化燃烧技术用于实际工程系统的可行性与经济效益。
Reverse flow reactor (RFR) is an integration of regenerative heat exchanger and fixed bed, in which flow direction is periodically changed. Applying such forced unsteady state operation (FUSO), a hot zone is trapped in the central catalytic section, which suits for exothermal catalytic reaction with low inlet concentration or reversible exothermal reaction with mild reaction heat release. Thus an increase in reactant conversion or product selectivity can be expected. This paper presents experimental and numerical results of the behavior of a bench-scale RFR, which is considered as a proper technology for decontaminating lean volatile organic compounds (VOCs) in waste gas. Effects of operation conditions on reactor behavior and corresponding control strategies when reactor stability is impaired are discussed.
A bench-scale RFR is built up, on which pressure drop through the reactor is studied. The results show that with periodic flow reversal, pressure drop of the reactor changes periodically. It takes several seconds to get a stable flow condition in the reactor soon after the flow reversal. However, effect of such temporary states on reactor behavior is rather since it is very short comparing to flow reversal time. Total pressure drop through the reactor can be calculated by Ergun equation very well, based on regression of experimental data, which means the pressure drop shows a quadratic increase of superficial velocity and a liner increase of bed depth.
Effects of operation parameters on reactor behavior are discussed, taking methane or benzene as model reactant. Temperature in the reactor varies periodically with flow reversal, while conversions of VOCs are all above98%if an auto-thermal operation is maintainded. Little NOx is detected. Basically, increasing inlet combustibles concentration or shortening flow reversal time will result in a higher thermal level and wider temperature plateau in reactor, which increase the VOCs conversion as well. Effect of superficial velocity is co-effect of heat release and convection. When binary mixture of methane and benzene is combusted in RFR, thermal level in reactor increases with the increasing of methane portion. Conversion of benzene is above95%. To eliminate the possibility of reactor thermal run away, decreasing inlet concentration or lengthening flow reversal time are all feasible ways. While using electrical heater or adding auxiliary fuel can increase reactor thermal lever, avoiding reactor extinction. But if methane is added as auxiliary fuel, large amount of methane is needed.
A one-dimensional heterogeneous is built up. Good accordance between simulation and experimental results are acquired.
Effect of reactor wall, transport parameters and reaction kinetics are discussed, based on numerical simulation. Moving range of heat wave is chosen as criterion when comparing effects of various operation parameters on reactor behavior. With parameters applied in this study, following optimum range of operation parameters are proposed, with superficial velocity of0.2～0.4m·s-1, moving range of heat wave taking20～40%of catalytic bed length and a inert packing taking20～40%of total reactor. Within this range, reactor operates more stable and lower minimum inlet concentration is required in maintaining auto-thermal operation.
Effect of periodic inlet concentration is studied. The results show that reactor stability is impaired in such situation, decreasing of reactor thermal level may even cause reactor extinction. Adjusting flow reversal time turns out to be a proper way in maintaining reactor stability. Based on experimental and numerical results, flow reversal time is regarded as characteristic response time of the reaction system. The reason why synchronizing between periodic inlet variation cycle and flow reversal cycle leads to dramatic maximum temperature variation is explained adopting harmonic analysis. According to this theory, the feasibility of changing system characteristic response time in maintaining stable operation is verified by numerical simulation.
With the results acquired in experiments and numerical simulation, a industrial scale reverse flow reactor for purifying waste gas flow of60000m·3h-1is designed, including system feasibility and economical analysis.
引文
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