催化裂化反应再生系统流动与反应耦合模拟
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摘要
本论文首先根据实验室小冷模装置(H=3.0m,D=0.012m)的实验数据(以空气及FCC(RHZ-300)催化剂为流化介质,表观气速U o为2.95～3.44 m /s ,固体质量通量Gs为23～40 kg /m 2s )建立了一个可预测的CFB提升管数学模型。计算及实验数据均表明:(a)在表观气速一定的情况下,轴向平均空隙率随固体循环通量的增加而减小;(b)在固体循环通量一定的情况下,轴向平均空隙率随表观气速的增大而增大;(c)在表观气速一定的情况下,整个提升管压降随固体循环通量的增大而增大,尤其是提升管底部变化最为明显。
模型将CFB提升管轴向分两段进行建模:底部加速段—即从固体颗粒入口处到被加速到一个不变的上行速度段及充分发展段—即流动特性均不再随提升管高度变化,从加速段结束处直到提升管出口段。模型假设提升管内气固两相呈环-核流结构,模型的输入参数包括提升管操作条件(如固体循环通量、表观气速)、提升管几何尺寸和流化介质的物理属性。同时,该模型可以很容易地与反应动力学模型耦合进行过程模拟。
其次,为了适应气体体积膨胀的反应过程,建立了变气速循环流化床流体力学模型,并采用其特例定气速实验数据进行了验证,结果表明数学模型完全可靠。
最后,采用该变气速流体力学模型结合四集总反应动力学模型建立了适合于FCC提升管的流动反应耦合模型,在模拟的小提升管(H=3.0m,D=0.012m)中计算表明:(a)原料油VGO通过3m长的提升管的最终转化率为93%。中间产物汽油在大约1m处就达到了最大值(约57%),之后随着二次反应的深入而逐渐下降,最终出口收率43%左右。C1-C4气体及焦炭则随着反应的加深而不断上升,出口收率分别为约40%和10%。(b)颗粒与气相两相温度分布规律:入口处,由于裂化反应剧烈,大量吸热,导致催化剂温度迅速下降,油汽温度迅速上升,大约在提升管高度的三分之一处,两相温度基本达到平衡。(c)催化剂颗粒在提升管底部有大量聚集,提升管上部空隙率很快达到一个定值。(d)从入口到出口,整个模拟提升管压降大约在8.6kPa。
此外,尝试建立了常规单段逆式再生器的烧焦反应模型。将再生器按拟均相两区模型进行建模,即密相床和自由沉降区。模拟计算了再生器内催化剂含碳随时间的动态变化规律、催化剂碳含量随再生器位置的分布规律、烟道气中氧,一氧化碳,二氧化碳等组分相对于再生空气/烟道气的摩尔比率分布规律等。
In the present study, based on the data from a bench scale riser (H=3.0m, D=0.012m, air and FCC catalyst are used as fluidizing agent, superficial velocity U0=2.95~3.44m/s, solid flux Gs=23~40kg/m2s). Firstly, a predictive mathematical model is proposed. The model calculation and experimental data shown: (a) Axial voidage increases with superficial velocity and decreases with the solid flux; (b) Higher solid volume fraction along riser in small scale riser than that in large scale one in the similar condition, especially in the bottom zone; (c) With the same superficial gas velocity, pressure gradient along the riser increases with the solid flux.
The proposed model assumes the CFB riser to be axially composed of two regions: an acceleration zone at the riser base, where solids re-injected from a standpipe are accelerated to a constant upward velocity, and a fully-developed region, where the flow characteristics are invariant with height, extending from the end of the acceleration region to the rise exit. The model postulates the existence of core-annulus type of flow structure and is based on both fundamental principles and empirical relationships. The input parameters to the model including the riser operate conditions (solids circulation flux and gas superficial velocity), riser geometry and gas and solids physical properties. What’s more, it can be easily coupled to kinetic models for process simulation.
Secondly, in order to couple the model with gas expanded reaction, a“variable-superficial velocity”hydrodynamic model was established for CFB riser, and applied the model to predict normal experimental data, it further confirmed the reliability of the proposed model. Finally, coupling the variable-superficial velocity hydrodynamic model with four lumps kinetic model, a hydro-kinetic model was established for FCC riser. The simulation proposed a riser reactor with 3 meter in height and 0.012 meter in diameter. The predictive results shown: (a) The conversion of the feedstock (VGO) is 93% through the 3-meter riser reactor, and most reaction take place in the initial third height of the riser. Intermediate product gasoline reach a peak (about 57%) at 1m, then gradually decreased for the secondary reaction. Final yield is 43% at the exit. As the final product, C1-C4 and coke final yield are 40% and 10%, respectively. (b) Two phase temperature distribution: at the inlet, the catalyst temperature declined for the fierce absorbs heat of catalytic reaction. And for feedstock (VGO), it fast increased to the balance with catalyst at one-third length of riser. (c) It shown that catalyst particles clustered in the bottom, but soon be accelerated and a constant average voidage is obtained in the upper section. (d) From the entrance to the exit, absolute pressure is decline, the whole riser pressure drop about 8.6kPa.
Besides, a conventional single-stage reverse-type regenerator is considered in the present thesis. The proposed model assumes the regenerator to be axially composed of two regions: dense bed, where majority of the catalyst are located and coke burning reactions take place, and freeboard, where a few ejected catalyst are captived by gravity and cyclones and after-burning take place. The model is used to simulation the coke concentration on catalyst against residence time, the coke concentration on regenerated catalyst against the height of regenerator, and the molar ratio of oxygen, carbon monoxide, carbon dioxide to regenerate air and/or to total stack gas along the regenerator.
模型将CFB提升管轴向分两段进行建模:底部加速段—即从固体颗粒入口处到被加速到一个不变的上行速度段及充分发展段—即流动特性均不再随提升管高度变化,从加速段结束处直到提升管出口段。模型假设提升管内气固两相呈环-核流结构,模型的输入参数包括提升管操作条件(如固体循环通量、表观气速)、提升管几何尺寸和流化介质的物理属性。同时,该模型可以很容易地与反应动力学模型耦合进行过程模拟。
其次,为了适应气体体积膨胀的反应过程,建立了变气速循环流化床流体力学模型,并采用其特例定气速实验数据进行了验证,结果表明数学模型完全可靠。
最后,采用该变气速流体力学模型结合四集总反应动力学模型建立了适合于FCC提升管的流动反应耦合模型,在模拟的小提升管(H=3.0m,D=0.012m)中计算表明:(a)原料油VGO通过3m长的提升管的最终转化率为93%。中间产物汽油在大约1m处就达到了最大值(约57%),之后随着二次反应的深入而逐渐下降,最终出口收率43%左右。C1-C4气体及焦炭则随着反应的加深而不断上升,出口收率分别为约40%和10%。(b)颗粒与气相两相温度分布规律:入口处,由于裂化反应剧烈,大量吸热,导致催化剂温度迅速下降,油汽温度迅速上升,大约在提升管高度的三分之一处,两相温度基本达到平衡。(c)催化剂颗粒在提升管底部有大量聚集,提升管上部空隙率很快达到一个定值。(d)从入口到出口,整个模拟提升管压降大约在8.6kPa。
此外,尝试建立了常规单段逆式再生器的烧焦反应模型。将再生器按拟均相两区模型进行建模,即密相床和自由沉降区。模拟计算了再生器内催化剂含碳随时间的动态变化规律、催化剂碳含量随再生器位置的分布规律、烟道气中氧,一氧化碳,二氧化碳等组分相对于再生空气/烟道气的摩尔比率分布规律等。
In the present study, based on the data from a bench scale riser (H=3.0m, D=0.012m, air and FCC catalyst are used as fluidizing agent, superficial velocity U0=2.95~3.44m/s, solid flux Gs=23~40kg/m2s). Firstly, a predictive mathematical model is proposed. The model calculation and experimental data shown: (a) Axial voidage increases with superficial velocity and decreases with the solid flux; (b) Higher solid volume fraction along riser in small scale riser than that in large scale one in the similar condition, especially in the bottom zone; (c) With the same superficial gas velocity, pressure gradient along the riser increases with the solid flux.
The proposed model assumes the CFB riser to be axially composed of two regions: an acceleration zone at the riser base, where solids re-injected from a standpipe are accelerated to a constant upward velocity, and a fully-developed region, where the flow characteristics are invariant with height, extending from the end of the acceleration region to the rise exit. The model postulates the existence of core-annulus type of flow structure and is based on both fundamental principles and empirical relationships. The input parameters to the model including the riser operate conditions (solids circulation flux and gas superficial velocity), riser geometry and gas and solids physical properties. What’s more, it can be easily coupled to kinetic models for process simulation.
Secondly, in order to couple the model with gas expanded reaction, a“variable-superficial velocity”hydrodynamic model was established for CFB riser, and applied the model to predict normal experimental data, it further confirmed the reliability of the proposed model. Finally, coupling the variable-superficial velocity hydrodynamic model with four lumps kinetic model, a hydro-kinetic model was established for FCC riser. The simulation proposed a riser reactor with 3 meter in height and 0.012 meter in diameter. The predictive results shown: (a) The conversion of the feedstock (VGO) is 93% through the 3-meter riser reactor, and most reaction take place in the initial third height of the riser. Intermediate product gasoline reach a peak (about 57%) at 1m, then gradually decreased for the secondary reaction. Final yield is 43% at the exit. As the final product, C1-C4 and coke final yield are 40% and 10%, respectively. (b) Two phase temperature distribution: at the inlet, the catalyst temperature declined for the fierce absorbs heat of catalytic reaction. And for feedstock (VGO), it fast increased to the balance with catalyst at one-third length of riser. (c) It shown that catalyst particles clustered in the bottom, but soon be accelerated and a constant average voidage is obtained in the upper section. (d) From the entrance to the exit, absolute pressure is decline, the whole riser pressure drop about 8.6kPa.
Besides, a conventional single-stage reverse-type regenerator is considered in the present thesis. The proposed model assumes the regenerator to be axially composed of two regions: dense bed, where majority of the catalyst are located and coke burning reactions take place, and freeboard, where a few ejected catalyst are captived by gravity and cyclones and after-burning take place. The model is used to simulation the coke concentration on catalyst against residence time, the coke concentration on regenerated catalyst against the height of regenerator, and the molar ratio of oxygen, carbon monoxide, carbon dioxide to regenerate air and/or to total stack gas along the regenerator.
引文
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