内循环气升式反应器流动行为与传质特性研究
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摘要
气升式反应器因其具有独特的优势在众多领域得到了广泛的应用，但是由于反应器内部多相流的流动和传质机理极其复杂，加上反应器结构、操作条件以及流体物性都会对流体流动特性和相间传质行为产生影响，在气升式反应器的设计、放大和操作等方面有很多问题尚未很好地解决。随着工业技术的迅速发展，业界对气升式反应器性能的要求也不断提高，因而如何设计更为高效的气升式反应器以及实现对反应器的优化操作成为迫切需要解决的问题。
本文以内循环气升式反应器为研究对象，考察了喷嘴结构和筛板结构对流体流动行为和相间传质特性的影响；基于轴向扩散模型建立了反应器的宏观传质模型，对动态气液传质过程进行了深入分析；初步研究了反应器内的压力波动与水力学行为之间的相互关系，提出了基于压力波动信号的流型辨识方法。
本文具体的研究内容以及得到的主要结论包括：
1.选取二喷嘴、旋切四喷嘴和O型分布器为研究对象，考察了喷嘴结构对流体流动和相间传质特性的影响。实验结果表明，在保证喷口出射气速相同的情况下，喷口直径较小的喷嘴产生的平均气泡直径较小，循环液速较大，有利于提高整体气含率和传质效率；通气量一定时，喷口数目越多会导致各喷口的气体出射速度越小，气体冲击破碎的效果越差，使得气液传质性能下降。综合实验数据，本文最终确定旋切四喷嘴为最优的喷嘴结构。
2.研究发现反应器内的流型变化对水力学行为影响很大，在均相流内，整体气含率和下降段液速都随表观气速的增大迅速增加，而在非均相流内，下降段液速基本趋于稳定，同时整体气含率的增加速度也变慢。体积氧传质系数随着表观气速的增加呈线性增加的趋势，提高表观气速对气泡比表面积（气液相界面积）的大小有显著影响，而对液膜侧氧传质系数的影响则有限。本文基于实验数据建立了预测不同流型、不同喷嘴结构下整体气含率和体积氧传质系数的经验关系式，同时根据物料守恒和压力平衡原则建立了预测下降段液速的流动模型，并对模型的有效性进行了验证。
3.考察了筛板结构对流体流动和传质行为的影响，发现筛板能够有效地破碎气泡，起到均布流场、强化传质的作用。在上升段内加装筛板后，反应器的性能有显著提高，整体气含率和体积氧传质系数均有大幅提升。筛孔直径和开孔率是筛板的重要结构参数，较小的筛孔直径和开孔率对于气含率的提升更有利，而较大的筛孔直径和开孔率强化传质的效果更明显。此外，筛板个数和安装位置也是影响反应器性能的重要因素，适量的增加筛板的数目对气液传质更有利，筛板安装在上升段下部效果更好。本文基于实验数据建立了预测不同筛板结构参数下整体气含率和体积氧传质系数的经验关系式，结合物料守恒和压力平衡原则建立了预测有筛板情况下下降段液速的流动模型，并验证了模型的有效性。
4.将带源相的轴向扩散模型应用于反应器内的气相和液相，建立了内循环气升式反应器的宏观传质模型。本文借助有限差分法将传质模型中的偏微分方程转化为差分方程，提出了模型的数值迭代求解方法；实验验证了模型的有效性，并结合实验数据和模型仿真结果，对反应器内的动态气液传质过程进行了详细阐述，证实了所研究的反应器具有良好的混合和传质特性；基于仿真结果得出的结论，对气液传质模型进行了简化，并通过坐标变换法求得了简化模型的解析解，计算结果表明该简化模型能较好地预测溶氧浓度的整体变化趋势。
5.研究了气升式反应器内的压力波动现象，探讨了反应器内压力波动的来源，并根据反应器内不同波源所产生的压力波动特性的差异将其划分为全局压力波动和局部压力波动两类；利用相关分析将压力波动信号分解为相关、联合非相关、自非相关三部分，各部分分别表征不同性质的波源产生的压力波动，并进一步考察了各部分所占的能量分率随表观气速的演化与反应器内流型转变之间的关系，证实了压力波动信号能够表征流型的转变；通过功率谱分析和相关分析研究了不同流型内压力波动信号的频率特征与水力学行为之间的相互关系。
6.对基于压力波动信号的流型辨识方法进行了深入研究，提出了流型辨识的新方法。本文分别利用小波变换、Hilbert-Huang变换、高阶统计量、Wigner-Ville分布以及混沌、分形理论对压力波动信号进行分析，提取出了压力信号中所蕴含的与流型相关的特征；通过采用小波熵、平均双谱、广义平均频率、Hurst指数、混沌特征参数作为表征流型转变的特征量，成功识别出反应器内的三种基本流型，为基于压力波动信号的流型辨识方法提供了新的研究思路。
Airlift reactors have been widely applied in chemical andbiotechnological industries due to their special advantages. However, becauseof the complexity of hydrodynamics and mass transfer in the reactor, togetherwith the influences of reactor structure, operating conditions and physicalproperties, there are still many remaining problems in designing, scaleup andoperating of the reactor. The demands on airlift reactors are increasing withthe development of industrial technologies. Thus, how to design an airliftreactor with high performance and realize the operation optimization of airliftreactors are key problems needing to be solved.
This work focuses on the hydrodynamics and mass transfercharacteristics in an internal loop airlift reactor. The influences of reactorstructures, such as sparger structure and sieve plate, on hydrodynamicbehaviors and mass transfer in the reactor were investigated. A macro masstransfer model of the reactor was established based on the axial dispersionmodel. The dynamic mass transfer process between gas and liquid phases wasanalyzed based on experimental data and simulation results. The pressurefluctuation phenomenon in the airlift reactor was studied and the relationshipbetween pressure fluctuations and hydrodynamic behaviors were revealed.Several new flow regime identification methods based on the pressurefluctuation signal were proposed.
The research content and main conclusions of this study including:
1. The influences of the sparger structure on hydrodynamics and masstransfer in the reactor were investigated. Three different spargers, namely2-orifice nozzle, rotary-cut4-orifice nozzle and O-ring distributor, were tested.It’s found that under the precondition of the same gas outlet velocity of eachorifice, the sparger with the smaller orifice diameter was more efficient for themass transfer, because it produced a smaller mean bubble diameter but a higher liquid circulation velocity, and therefore a higher volumetric masstransfer coefficient. At the given airflow rate, the lager number of orificesleads to a low gas outlet velocity of each orifice, which weakens the impactbetween gas and liquid phases, resulting in the decrease of mass transferefficiency. The rotary-cut4-orifice nozzle was confirmed to be the bestsparger.
2. The flow regime transitions have a large influence on hydrodynamicbehaviors. In the homogeneous flow, the overall gas holdup and thedowncomer liquid velocity increased with the superficial gas velocity, whilethe downcomer liquid velocity tended to be stable and the increase of gasholdup slowed down in the heterogeneous flow. The volumetric mass transfercoefficient almost increased linearly with the superficial gas velocity. Thesuperficial gas velocity strongly affected the specific interfacial area, whilehad less effect on the liquid-side mass transfer coefficient. Empiricalcorrelations were proposed to predict the gas holdup and the volumetric masstransfer coefficient for different spargers in different flow regimes. Based onthe material conservation and pressure balance principles, a fluid model wasestablished to predict the liquid velocity in the downcomer, and itseffectiveness was validated by experiment data.
3. Effects of the sieve plate on flow and mass transfer characteristics inthe reactor were studied. It’s found that the sieve plate played an importantrole in breaking up bubbles, and thus made the flow field more uniform andenhanced the mass transfer efficiency. The installing of sieve plates in theriser could significantly enhance gas holdup and volumetric mass transfercoefficient. The sieve pore diameter and the free area ratio are importantdesign parameters of the sieve plate. Smaller sieve pore diameter and freearea ratio were more benefit to increase the gas holdup, while larger sievepore diameter and free area ratio were more efficient in enhancing the masstransfer efficiency. Moreover, the number and mounting position of the sieveplate also have strong effect on the performance of the reactor. The resultsindicated that the mass transfer coefficient was larger when more sieve plates were used. The installing of the sieve plate at the bottom section of the riserwas found to be more efficient. Empirical correlations were proposed topredict gas holdup and volumetric mass transfer coefficient for different sievestructure parameters. A fluid model was established to predict the downcomerliquid velocity in the airlift reactor with sieve plates.
4. A macro mass transfer model of the airlift reactor was established byapplying the axial dispersion model to gas and liquid phases. The partialdifferential equations of mass transfer model were transformed to differenceequations using the finite difference method, and a numerical method wasdeveloped to solve the mathematical model. Experiments were carried out tovalidate the effectiveness of the model. Based on experiment data andnumerical simulation results, the dynamic mass transfer process in the reactorwas illustrated in details. Based on the conclusion obtained from numericalresults, the mass transfer model was further simplified and the analyticalsolution of the simplified model was obtained by using a coordinate transformmethod. The results indicated that the simplified model could well predict thedissolved oxygen concentration when axial dispersion coefficients and axialconcentration gradients in the reactor were negligible.
5. The origin of pressure fluctuations in airlift reactors was discussed.The pressure fluctuations in the reactor were divided into two categories:global pressure fluctuations and local pressure fluctuations. Based on thecoherence analysis, the pressure signal was decomposed into three differentparts: coherent part, joint incoherent part and exclusive incoherent part. Eachpart was related to pressure fluctuations from different sources. Therelationship between evolution of energy ratios of these three parts with thesuperficial gas velocity and flow regime transitions in the reactor wasinvestigated. The results indicated that the pressure signal was capable torepresent flow regime transitions. The power spectral and coherence analysismethods were applied to study the relationship between pressure fluctuationsand hydrodynamic behaviors in different flow regimes.
6. The flow regime identification based on pressure fluctuation signals was deeply investigated and several new flow regime identification methodswere proposed. The wavelet transform, Hilbert-Huang transform, higher orderstatistics, Wigner-Ville distribution, chaos and fractal theories were applied toanalyze pressure fluctuation signals, and thus the flow regime characteristicswere extracted from the pressure signal. By using the wavelet entropy,average bispectrum, generalized average frequency, Hurst exponent andchaotic parameters as characteristic quantities, the three typical flow regimesin the reactor were successfully identified. These results provide a newthought for the flow regime identification based on pressure fluctuationsignals.
本文以内循环气升式反应器为研究对象，考察了喷嘴结构和筛板结构对流体流动行为和相间传质特性的影响；基于轴向扩散模型建立了反应器的宏观传质模型，对动态气液传质过程进行了深入分析；初步研究了反应器内的压力波动与水力学行为之间的相互关系，提出了基于压力波动信号的流型辨识方法。
本文具体的研究内容以及得到的主要结论包括：
1.选取二喷嘴、旋切四喷嘴和O型分布器为研究对象，考察了喷嘴结构对流体流动和相间传质特性的影响。实验结果表明，在保证喷口出射气速相同的情况下，喷口直径较小的喷嘴产生的平均气泡直径较小，循环液速较大，有利于提高整体气含率和传质效率；通气量一定时，喷口数目越多会导致各喷口的气体出射速度越小，气体冲击破碎的效果越差，使得气液传质性能下降。综合实验数据，本文最终确定旋切四喷嘴为最优的喷嘴结构。
2.研究发现反应器内的流型变化对水力学行为影响很大，在均相流内，整体气含率和下降段液速都随表观气速的增大迅速增加，而在非均相流内，下降段液速基本趋于稳定，同时整体气含率的增加速度也变慢。体积氧传质系数随着表观气速的增加呈线性增加的趋势，提高表观气速对气泡比表面积（气液相界面积）的大小有显著影响，而对液膜侧氧传质系数的影响则有限。本文基于实验数据建立了预测不同流型、不同喷嘴结构下整体气含率和体积氧传质系数的经验关系式，同时根据物料守恒和压力平衡原则建立了预测下降段液速的流动模型，并对模型的有效性进行了验证。
3.考察了筛板结构对流体流动和传质行为的影响，发现筛板能够有效地破碎气泡，起到均布流场、强化传质的作用。在上升段内加装筛板后，反应器的性能有显著提高，整体气含率和体积氧传质系数均有大幅提升。筛孔直径和开孔率是筛板的重要结构参数，较小的筛孔直径和开孔率对于气含率的提升更有利，而较大的筛孔直径和开孔率强化传质的效果更明显。此外，筛板个数和安装位置也是影响反应器性能的重要因素，适量的增加筛板的数目对气液传质更有利，筛板安装在上升段下部效果更好。本文基于实验数据建立了预测不同筛板结构参数下整体气含率和体积氧传质系数的经验关系式，结合物料守恒和压力平衡原则建立了预测有筛板情况下下降段液速的流动模型，并验证了模型的有效性。
4.将带源相的轴向扩散模型应用于反应器内的气相和液相，建立了内循环气升式反应器的宏观传质模型。本文借助有限差分法将传质模型中的偏微分方程转化为差分方程，提出了模型的数值迭代求解方法；实验验证了模型的有效性，并结合实验数据和模型仿真结果，对反应器内的动态气液传质过程进行了详细阐述，证实了所研究的反应器具有良好的混合和传质特性；基于仿真结果得出的结论，对气液传质模型进行了简化，并通过坐标变换法求得了简化模型的解析解，计算结果表明该简化模型能较好地预测溶氧浓度的整体变化趋势。
5.研究了气升式反应器内的压力波动现象，探讨了反应器内压力波动的来源，并根据反应器内不同波源所产生的压力波动特性的差异将其划分为全局压力波动和局部压力波动两类；利用相关分析将压力波动信号分解为相关、联合非相关、自非相关三部分，各部分分别表征不同性质的波源产生的压力波动，并进一步考察了各部分所占的能量分率随表观气速的演化与反应器内流型转变之间的关系，证实了压力波动信号能够表征流型的转变；通过功率谱分析和相关分析研究了不同流型内压力波动信号的频率特征与水力学行为之间的相互关系。
6.对基于压力波动信号的流型辨识方法进行了深入研究，提出了流型辨识的新方法。本文分别利用小波变换、Hilbert-Huang变换、高阶统计量、Wigner-Ville分布以及混沌、分形理论对压力波动信号进行分析，提取出了压力信号中所蕴含的与流型相关的特征；通过采用小波熵、平均双谱、广义平均频率、Hurst指数、混沌特征参数作为表征流型转变的特征量，成功识别出反应器内的三种基本流型，为基于压力波动信号的流型辨识方法提供了新的研究思路。
Airlift reactors have been widely applied in chemical andbiotechnological industries due to their special advantages. However, becauseof the complexity of hydrodynamics and mass transfer in the reactor, togetherwith the influences of reactor structure, operating conditions and physicalproperties, there are still many remaining problems in designing, scaleup andoperating of the reactor. The demands on airlift reactors are increasing withthe development of industrial technologies. Thus, how to design an airliftreactor with high performance and realize the operation optimization of airliftreactors are key problems needing to be solved.
This work focuses on the hydrodynamics and mass transfercharacteristics in an internal loop airlift reactor. The influences of reactorstructures, such as sparger structure and sieve plate, on hydrodynamicbehaviors and mass transfer in the reactor were investigated. A macro masstransfer model of the reactor was established based on the axial dispersionmodel. The dynamic mass transfer process between gas and liquid phases wasanalyzed based on experimental data and simulation results. The pressurefluctuation phenomenon in the airlift reactor was studied and the relationshipbetween pressure fluctuations and hydrodynamic behaviors were revealed.Several new flow regime identification methods based on the pressurefluctuation signal were proposed.
The research content and main conclusions of this study including:
1. The influences of the sparger structure on hydrodynamics and masstransfer in the reactor were investigated. Three different spargers, namely2-orifice nozzle, rotary-cut4-orifice nozzle and O-ring distributor, were tested.It’s found that under the precondition of the same gas outlet velocity of eachorifice, the sparger with the smaller orifice diameter was more efficient for themass transfer, because it produced a smaller mean bubble diameter but a higher liquid circulation velocity, and therefore a higher volumetric masstransfer coefficient. At the given airflow rate, the lager number of orificesleads to a low gas outlet velocity of each orifice, which weakens the impactbetween gas and liquid phases, resulting in the decrease of mass transferefficiency. The rotary-cut4-orifice nozzle was confirmed to be the bestsparger.
2. The flow regime transitions have a large influence on hydrodynamicbehaviors. In the homogeneous flow, the overall gas holdup and thedowncomer liquid velocity increased with the superficial gas velocity, whilethe downcomer liquid velocity tended to be stable and the increase of gasholdup slowed down in the heterogeneous flow. The volumetric mass transfercoefficient almost increased linearly with the superficial gas velocity. Thesuperficial gas velocity strongly affected the specific interfacial area, whilehad less effect on the liquid-side mass transfer coefficient. Empiricalcorrelations were proposed to predict the gas holdup and the volumetric masstransfer coefficient for different spargers in different flow regimes. Based onthe material conservation and pressure balance principles, a fluid model wasestablished to predict the liquid velocity in the downcomer, and itseffectiveness was validated by experiment data.
3. Effects of the sieve plate on flow and mass transfer characteristics inthe reactor were studied. It’s found that the sieve plate played an importantrole in breaking up bubbles, and thus made the flow field more uniform andenhanced the mass transfer efficiency. The installing of sieve plates in theriser could significantly enhance gas holdup and volumetric mass transfercoefficient. The sieve pore diameter and the free area ratio are importantdesign parameters of the sieve plate. Smaller sieve pore diameter and freearea ratio were more benefit to increase the gas holdup, while larger sievepore diameter and free area ratio were more efficient in enhancing the masstransfer efficiency. Moreover, the number and mounting position of the sieveplate also have strong effect on the performance of the reactor. The resultsindicated that the mass transfer coefficient was larger when more sieve plates were used. The installing of the sieve plate at the bottom section of the riserwas found to be more efficient. Empirical correlations were proposed topredict gas holdup and volumetric mass transfer coefficient for different sievestructure parameters. A fluid model was established to predict the downcomerliquid velocity in the airlift reactor with sieve plates.
4. A macro mass transfer model of the airlift reactor was established byapplying the axial dispersion model to gas and liquid phases. The partialdifferential equations of mass transfer model were transformed to differenceequations using the finite difference method, and a numerical method wasdeveloped to solve the mathematical model. Experiments were carried out tovalidate the effectiveness of the model. Based on experiment data andnumerical simulation results, the dynamic mass transfer process in the reactorwas illustrated in details. Based on the conclusion obtained from numericalresults, the mass transfer model was further simplified and the analyticalsolution of the simplified model was obtained by using a coordinate transformmethod. The results indicated that the simplified model could well predict thedissolved oxygen concentration when axial dispersion coefficients and axialconcentration gradients in the reactor were negligible.
5. The origin of pressure fluctuations in airlift reactors was discussed.The pressure fluctuations in the reactor were divided into two categories:global pressure fluctuations and local pressure fluctuations. Based on thecoherence analysis, the pressure signal was decomposed into three differentparts: coherent part, joint incoherent part and exclusive incoherent part. Eachpart was related to pressure fluctuations from different sources. Therelationship between evolution of energy ratios of these three parts with thesuperficial gas velocity and flow regime transitions in the reactor wasinvestigated. The results indicated that the pressure signal was capable torepresent flow regime transitions. The power spectral and coherence analysismethods were applied to study the relationship between pressure fluctuationsand hydrodynamic behaviors in different flow regimes.
6. The flow regime identification based on pressure fluctuation signals was deeply investigated and several new flow regime identification methodswere proposed. The wavelet transform, Hilbert-Huang transform, higher orderstatistics, Wigner-Ville distribution, chaos and fractal theories were applied toanalyze pressure fluctuation signals, and thus the flow regime characteristicswere extracted from the pressure signal. By using the wavelet entropy,average bispectrum, generalized average frequency, Hurst exponent andchaotic parameters as characteristic quantities, the three typical flow regimesin the reactor were successfully identified. These results provide a newthought for the flow regime identification based on pressure fluctuationsignals.
引文
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