整体式结构化催化剂合成异丙苯的反应过程强化
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摘要
异丙苯是一种重要的有机化工原料,用途十分广泛。本文采用单元模块模拟CFD、过程模拟Aspen Plus和Pro Ⅱ以及实验相结合的方法研究了苯与丙烯在整体式结构化催化剂合成异丙苯的反应过程强化及分离工段的能耗分析,考察了两类整体式结构化催化剂结构-性能(压降、传质、传热、丙烯转化率、异丙苯选择性、反应有效因子等)关系。
首先,采用Pro Ⅱ和Aspen Plus过程模拟软件对颗粒催化剂固定床反应器合成异丙苯工艺流程进行优化模拟计算。以降低异丙苯流程中分离工段单位产品的能耗为目标本文逐步提出流程优化方案：在分离工段的二异丙苯塔增加一个侧线采出以回收三异丙苯,从而实现过程的节能减排；采用泡点反应器代替原固定床反应器进行苯丙烯烷基化反应；同时采用泡点反应器和增加二异丙苯塔侧线采出的方法合成异丙苯；最后提出采用固定床催化精馏塔合成异丙苯。
第二,以空气-水逆流流动为研究对象采用实验和CFD数值模拟相结合的方法对两种开放错流整体式结构化催化剂(BH-1和BH-2型)的流体力学性能进行了研究,结果表明开放错流结构具有明显的低压降,相同操作条件下气体通过单位长度催化剂的压降比普通颗粒催化剂降低1-3个数量级。同时考察了几何结构参数(波纹板倾斜角、高径比及反应／分离面积比)对其流体力学性能的影响,研究结果表明,对于不同波纹板倾斜角时,单位长度催化剂的压降大小顺序为30°<30-45-300<45-30-45°<45°,液相传质系数KLa大小顺序为45°>45-30-45°>30-45-30°>30°；不同高径比(保持其直径不变,改变催化剂的高度)时,空气-水逆流流动通过单位长度催化剂的压降大小顺序为0.20m<0.15m<0.10m,液相传质系数KLa从大到小依次为0.10m>0.15m>0.20m；对于BH-1型开放错流整体式结构化催化剂改变不同反应/分离区域面积比(保持其分离区域不变,改变催化剂捆包厚度)时,单位长度催化剂的压降大小顺序为6mm<10mm<14mm,液相传质系数KLa从大到小依次为6mm>10mm>14mm；可见高传质性能将意味着高的压力损失,开放错流结构整体式结构化催化剂具有结构参数可调性,在实际应用中可以根据具体情况来设计更加合理的结构。
第三,将BH型开放错流整体式结构化催化剂(BH-1)应用于异丙苯的合成过程中,通过建立可靠的数学模型来考察苯与丙烯烷基化过程中整体式结构化催化剂的传递和反应特性,结果表明最佳反应条件为反应温度160℃,进料苯烯摩尔比为4.0。进一步通过数学模型,定量的描述了整体式结构化催化剂结构-性能(动量传递、质量传递、热量传递和反应特性)之间的关系。结果表明两种折线式波纹板(30-45-30°和45-30-45°)表现出高丙烯转化率、高异丙苯选择性和反应有效因子；低高径比有利于提高质量传递和反应的有效因子,但同时也增大了压降降低了异丙苯的选择性；反应/分离面积比越低压降越小,同时异丙苯选择性和反应有效因子越高,但却不利于总的丙烯质量传递和转化率的提高。
最后,通过实验和模拟相结合的方法考察了蜂窝式结构化催化剂在苯与丙烯烷基化反应时的传递和反应特性,建立了可靠的数学模型并采用此数学模型考察了不同通道结构形状(圆形、正方形、长方形、六边形和三角形)对其特性(单位催化剂压降、传质特性Nu、修伍德准数Sh、丙烯转化率x和异丙苯的选择性S、反应有效因子η、坦克莱准数Da)的影响,结果表明蜂窝式结构化催化剂具有低压降、高异丙苯选择性和高反应有效因子的特性,同时对比不同结构通道形状,综合考虑压降和异丙苯的特性正三角形和矩形结构为优。从工程角度出发,泡点反应器和整体式结构化催化剂联合使用能同时降低压降和反应分离过程的能量消耗。本文进一步对比了采用三种不同类型催化剂(蜂窝式结构化催化剂、BH型开放错流整体式结构化催化剂和YSBH颗粒催化剂)和泡点反应器耦合合成异丙苯时,发现采用蜂窝式结构化催化剂时分离工段能耗最低。
Cumene (or isopropylbenzene) is an important starting material for the production of acetone and phenol. This work investigated the transfer and reaction performances and the energy consumptions for the alkylation reaction of benzene with propylene to cumene over structured catalysts using the combination the CFD simulation, Aspen Plus, Pro II, and experimental methods. Furthermore, the relation between geometric parameters and reactor performances (the pressure drop, mass transfer, heat transfer, propylene conversion, cumene selectivity, effectiveness factor, and so on) was identified using CFD models.
Firstly, due to high energy consumption brought by high feeding molar ratio of benzene to propylene, an optimized process design has been developed and is presented. First, a side-stream was added to the DIPB distillation column to recover some triisopropylbenzene (TIPB), resulting in a decrease of the energy consumption per product. On the other hand, if the original fixed-bed reactor is replaced by a bubble-point reactor, the total heat duty on condensers and reboilers will decrease by18.5and22.8%, respectively. Then, a fixed-bed catalytic distillation (FCD) column was proposed for producing cumene. The improvement of FCD column was done by carrying out alkylation and transalkylation reactions simultaneously in a single column for producing cumene, with the result that investment of equipment for transalkylation is reduced and the process is simplified. Finally, with the combination of the improved DIPB column and FCD process, the heat duty was found to be the lowest.
Secondly, two types of structured catalytic packings (i.e. BH-1and BH-2types) were involved, and the relationship between geometric configuration and performance of pressure drop and mass transfer coefficients for BH-1and BH-2types was identified by means of the combination of experiments and computational fluid dynamics (CFD). The results showed that under the same operating conditions pressure drops for BH-1and BH-2types were significantly lower than those for conventional fixed-bed reactor packed with pellet catalyst particles by one to three orders of magnitude. Two kinds of transition structures were proposed and the calculated results revealed that they were favorable when considering pressure drop and mass transfer coefficient together. Furthermore, it was found that a low ratio of packing height to diameter was favorable for increasing mass transfer coefficient, but leads to increasing pressure drop like common structured packings; a low area ratio of separation to reaction region for BH-1type would increase mass transfer coefficient and decrease pressure drop simultaneously.
Thirdly, a three-dimensional (3D) mathematical model was established to determine the optimum operating conditions and to examine the reactor performance when traditional catalyst pellets were replaced with BH structured catalytic packings for benzene alkylation with propylene. It was found that the optimum operating conditions were the reaction temperature of160℃and the molar ratio of benzene to propylene in the feed of4.0. In this work, we also explored the relationship between the geometric configuration and the reactor performance. The momentum transfer (pressure drop), heat transfer (Nu number), mass transfer (Sh number), propylene conversion, cumene selectivity, and effectiveness factor were determined for different geometric configurations, which included changes in the corrugation angle, ratio of the packing height to the diameter, and ratio of the areas of the reaction and open-channel regions. Two new types of transition or wave-like structures (30-45-30°and45-30-45°), which resulted in a higher propylene conversion, cumene selectivity and effectiveness factor, were adopted. Furthermore, the applicability of this new technology for benzene alkylation with propylene was verified in a pilot plant.
Finally, the transfer and reaction performances for benzene alkylation with propylene to produce cumene over monolith catalysts were investigated by means of the combination of experiments and computational fluid dynamics (CFDs). A three-dimensional (3D) mathematical model was established to identify the geometric configuration-performance relation so as to provide a comprehensive comparison of momentum transfer (pressure drop), heat transfer (Nu number), mass transfer (Sh number), and reaction performances (i.e. propylene conversion, cumene selectivity, and effectiveness factor) among monolith catalysts with five kinds of channel shapes (i.e. circle, hexagon, square, rectangle, and regular triangle). It was found that monolith catalyst exhibits the lower pressure drop, higher cumene selectivity and higher effectiveness factor; and regular triangle or rectangle channel is optimum when considering pressure drop and cumene selectivity together. Furthermore, the advantages of monolith catalyst can lead to the lowest energy consumption for the whole process.
首先,采用Pro Ⅱ和Aspen Plus过程模拟软件对颗粒催化剂固定床反应器合成异丙苯工艺流程进行优化模拟计算。以降低异丙苯流程中分离工段单位产品的能耗为目标本文逐步提出流程优化方案：在分离工段的二异丙苯塔增加一个侧线采出以回收三异丙苯,从而实现过程的节能减排；采用泡点反应器代替原固定床反应器进行苯丙烯烷基化反应；同时采用泡点反应器和增加二异丙苯塔侧线采出的方法合成异丙苯；最后提出采用固定床催化精馏塔合成异丙苯。
第二,以空气-水逆流流动为研究对象采用实验和CFD数值模拟相结合的方法对两种开放错流整体式结构化催化剂(BH-1和BH-2型)的流体力学性能进行了研究,结果表明开放错流结构具有明显的低压降,相同操作条件下气体通过单位长度催化剂的压降比普通颗粒催化剂降低1-3个数量级。同时考察了几何结构参数(波纹板倾斜角、高径比及反应／分离面积比)对其流体力学性能的影响,研究结果表明,对于不同波纹板倾斜角时,单位长度催化剂的压降大小顺序为30°<30-45-300<45-30-45°<45°,液相传质系数KLa大小顺序为45°>45-30-45°>30-45-30°>30°；不同高径比(保持其直径不变,改变催化剂的高度)时,空气-水逆流流动通过单位长度催化剂的压降大小顺序为0.20m<0.15m<0.10m,液相传质系数KLa从大到小依次为0.10m>0.15m>0.20m；对于BH-1型开放错流整体式结构化催化剂改变不同反应/分离区域面积比(保持其分离区域不变,改变催化剂捆包厚度)时,单位长度催化剂的压降大小顺序为6mm<10mm<14mm,液相传质系数KLa从大到小依次为6mm>10mm>14mm；可见高传质性能将意味着高的压力损失,开放错流结构整体式结构化催化剂具有结构参数可调性,在实际应用中可以根据具体情况来设计更加合理的结构。
第三,将BH型开放错流整体式结构化催化剂(BH-1)应用于异丙苯的合成过程中,通过建立可靠的数学模型来考察苯与丙烯烷基化过程中整体式结构化催化剂的传递和反应特性,结果表明最佳反应条件为反应温度160℃,进料苯烯摩尔比为4.0。进一步通过数学模型,定量的描述了整体式结构化催化剂结构-性能(动量传递、质量传递、热量传递和反应特性)之间的关系。结果表明两种折线式波纹板(30-45-30°和45-30-45°)表现出高丙烯转化率、高异丙苯选择性和反应有效因子；低高径比有利于提高质量传递和反应的有效因子,但同时也增大了压降降低了异丙苯的选择性；反应/分离面积比越低压降越小,同时异丙苯选择性和反应有效因子越高,但却不利于总的丙烯质量传递和转化率的提高。
最后,通过实验和模拟相结合的方法考察了蜂窝式结构化催化剂在苯与丙烯烷基化反应时的传递和反应特性,建立了可靠的数学模型并采用此数学模型考察了不同通道结构形状(圆形、正方形、长方形、六边形和三角形)对其特性(单位催化剂压降、传质特性Nu、修伍德准数Sh、丙烯转化率x和异丙苯的选择性S、反应有效因子η、坦克莱准数Da)的影响,结果表明蜂窝式结构化催化剂具有低压降、高异丙苯选择性和高反应有效因子的特性,同时对比不同结构通道形状,综合考虑压降和异丙苯的特性正三角形和矩形结构为优。从工程角度出发,泡点反应器和整体式结构化催化剂联合使用能同时降低压降和反应分离过程的能量消耗。本文进一步对比了采用三种不同类型催化剂(蜂窝式结构化催化剂、BH型开放错流整体式结构化催化剂和YSBH颗粒催化剂)和泡点反应器耦合合成异丙苯时,发现采用蜂窝式结构化催化剂时分离工段能耗最低。
Cumene (or isopropylbenzene) is an important starting material for the production of acetone and phenol. This work investigated the transfer and reaction performances and the energy consumptions for the alkylation reaction of benzene with propylene to cumene over structured catalysts using the combination the CFD simulation, Aspen Plus, Pro II, and experimental methods. Furthermore, the relation between geometric parameters and reactor performances (the pressure drop, mass transfer, heat transfer, propylene conversion, cumene selectivity, effectiveness factor, and so on) was identified using CFD models.
Firstly, due to high energy consumption brought by high feeding molar ratio of benzene to propylene, an optimized process design has been developed and is presented. First, a side-stream was added to the DIPB distillation column to recover some triisopropylbenzene (TIPB), resulting in a decrease of the energy consumption per product. On the other hand, if the original fixed-bed reactor is replaced by a bubble-point reactor, the total heat duty on condensers and reboilers will decrease by18.5and22.8%, respectively. Then, a fixed-bed catalytic distillation (FCD) column was proposed for producing cumene. The improvement of FCD column was done by carrying out alkylation and transalkylation reactions simultaneously in a single column for producing cumene, with the result that investment of equipment for transalkylation is reduced and the process is simplified. Finally, with the combination of the improved DIPB column and FCD process, the heat duty was found to be the lowest.
Secondly, two types of structured catalytic packings (i.e. BH-1and BH-2types) were involved, and the relationship between geometric configuration and performance of pressure drop and mass transfer coefficients for BH-1and BH-2types was identified by means of the combination of experiments and computational fluid dynamics (CFD). The results showed that under the same operating conditions pressure drops for BH-1and BH-2types were significantly lower than those for conventional fixed-bed reactor packed with pellet catalyst particles by one to three orders of magnitude. Two kinds of transition structures were proposed and the calculated results revealed that they were favorable when considering pressure drop and mass transfer coefficient together. Furthermore, it was found that a low ratio of packing height to diameter was favorable for increasing mass transfer coefficient, but leads to increasing pressure drop like common structured packings; a low area ratio of separation to reaction region for BH-1type would increase mass transfer coefficient and decrease pressure drop simultaneously.
Thirdly, a three-dimensional (3D) mathematical model was established to determine the optimum operating conditions and to examine the reactor performance when traditional catalyst pellets were replaced with BH structured catalytic packings for benzene alkylation with propylene. It was found that the optimum operating conditions were the reaction temperature of160℃and the molar ratio of benzene to propylene in the feed of4.0. In this work, we also explored the relationship between the geometric configuration and the reactor performance. The momentum transfer (pressure drop), heat transfer (Nu number), mass transfer (Sh number), propylene conversion, cumene selectivity, and effectiveness factor were determined for different geometric configurations, which included changes in the corrugation angle, ratio of the packing height to the diameter, and ratio of the areas of the reaction and open-channel regions. Two new types of transition or wave-like structures (30-45-30°and45-30-45°), which resulted in a higher propylene conversion, cumene selectivity and effectiveness factor, were adopted. Furthermore, the applicability of this new technology for benzene alkylation with propylene was verified in a pilot plant.
Finally, the transfer and reaction performances for benzene alkylation with propylene to produce cumene over monolith catalysts were investigated by means of the combination of experiments and computational fluid dynamics (CFDs). A three-dimensional (3D) mathematical model was established to identify the geometric configuration-performance relation so as to provide a comprehensive comparison of momentum transfer (pressure drop), heat transfer (Nu number), mass transfer (Sh number), and reaction performances (i.e. propylene conversion, cumene selectivity, and effectiveness factor) among monolith catalysts with five kinds of channel shapes (i.e. circle, hexagon, square, rectangle, and regular triangle). It was found that monolith catalyst exhibits the lower pressure drop, higher cumene selectivity and higher effectiveness factor; and regular triangle or rectangle channel is optimum when considering pressure drop and cumene selectivity together. Furthermore, the advantages of monolith catalyst can lead to the lowest energy consumption for the whole process.
引文
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