Optimal design and control of reactive distillation process with component recycle for the synthesis of n-propyl propionate

doi:10.11949/0438-1157.20230967

Abstract

Abstract:

A reactive distillation process with component recycling is proposed to address the challenging operational issues for unfavorable volatility sequence in the reaction system. Taking the esterification of excess n-propanol with propionic acid to produce n-propyl propionate as an example, a reactive distillation process with n-propanol circulation was constructed. The pinch point of the binary vapor-liquid equilibrium of n-propyl propiate and n-propanol was determined by thermodynamic analysis, and the integrated process of reactive distillation was systematically studied to determine the purity of recycled n-propanol (X_ProOH). Using sequential optimization method, the operating parameters and structural parameters of the reactive distillation column and recovery column were determined with the minimum annual total cost (TAC) as the optimization objective. The results show that when X_ProOH=0.80, a trade-off between the reaction process of the reactive distillation tower and the separation process of the recovery tower is achieved, and the process parameters with minimum TAC are obtained. In addition, a composition/temperature-proportional control scheme is proposed to study the dynamic response performance of the closed-loop system when the disturbance of ±10% propionic acid feed flow is introduced.

Key words: reactive distillation, n-propyl propionate, circulation purity, optimization, control

摘要：

针对反应体系存在最不利挥发度序列的反应精馏难操作问题，提出带组分循环的反应精馏工艺，以过量正丙醇与丙酸酯化反应生产丙酸正丙酯为对象，构建了一种正丙醇循环的反应精馏工艺。通过热力学分析确定丙酸正丙酯和正丙醇二元体系存在夹点，系统研究了正丙醇循环纯度（X_ProOH）对反应精馏集成过程的影响，并以年度总成本（TAC）为优化目标，通过序贯优化法确定反应精馏塔及回收塔的操作参数和结构参数。结果表明，当X_ProOH=0.80时，达到反应精馏塔反应过程和回收塔分离过程之间的权衡，获得TAC最小的工艺过程参数。此外，进一步提出一种组成/温度-比例控制方案，研究了闭环系统中引入±10%丙酸进料流量扰动时动态响应性能，结果表明该控制方案具有较好的抗干扰能力。

关键词: 反应精馏, 丙酸正丙酯, 循环纯度, 优化, 控制

CLC Number:

TQ 225.24

Wuxiang LI, Yuyu SUN, Danyang LIU, Xinlei CAI, Jihai TANG, Yiping HUANG, Guowen ZHANG, Zhuxiu ZHANG, Xu QIAO. Optimal design and control of reactive distillation process with component recycle for the synthesis of n-propyl propionate[J]. CIESC Journal, 2023, 74(12): 4945-4955.

李武祥, 孙玉玉, 刘丹阳, 蔡鑫磊, 汤吉海, 黄益平, 张国雯, 张竹修, 乔旭. 带组分循环反应精馏合成丙酸正丙酯过程优化设计与控制[J]. 化工学报, 2023, 74(12): 4945-4955.

Figures/Tables 13

Fig.1 Flow chart of n-propyl propionate reactive distillation process

Table 1 Pre-exponential factors and activation energy of reaction rates

物理量	数值
$k 0 +$ /(kmol/(m³·s))	6.014×10⁶
$k 0 -$ /(kmol/(m³·s))	9.602×10⁵
$E 0 +$ /(kJ/mol)	59.63
$E 0 -$ /(kJ/mol)	64.15

Table 1 Pre-exponential factors and activation energy of reaction rates

物理量	数值
$k 0 +$ /(kmol/(m³·s))	6.014×10⁶
$k 0 -$ /(kmol/(m³·s))	9.602×10⁵
$E 0 +$ /(kJ/mol)	59.63
$E 0 -$ /(kJ/mol)	64.15

Table 2 UNIQUAC model parameters

i-j	a_ij	a_ji	b_ij	b_ji
ProAc-ProOH	0	0	183.915	-145.676
ProAc-H₂O	0	0	73.8	-244.8
ProOH-ProPro	0	0	-1.924	-87.25
ProOH-H₂O	1.838	-2.408	-668.969	620.785
ProPro-H₂O	6.751	1.905	-3267.486	-781.895
ProAc-ProPro	0	0	119.902	-229.392

Table 3 Boiling point and azeotropic data of the system at 1 atm

构成	类型	温度/℃		组成（摩尔基准）
构成	类型	文献值	计算值	文献值	计算值
ProOH-ProPro-H₂O	多相	86.20	86.41	0.350/0.130/0.520	0.273/0.140/0.587
ProOH-H₂O	均相	87.60	87.64	0.432/0.568	0.406/0.594
ProPro-H₂O	多相	90.00	89.10	0.350/0.650	0.333/0.667
ProAc-H₂O	均相	99.90	99.96	0.050/0.950	0.037/0.963
ProOH	—	97.20	97.20	—	—
ProAc	—	141.17	141.14	—	—
ProPro	—	122.60	122.40	—	—
H₂O	—	100.00	100.02	—	—

Fig.2 Residual curve of ProOH-ProPro-H2O at 1 atm

Fig.3 T-xy phase diagram of ProPro-ProOH at 1 atm

Fig.4 Flowchart of sequential optimization method

Fig.5 The economic impact of each parameter of RDC tower under different cycle purity

Fig.6 The economic impact of different cycle purities on the overall systeam

Table 4 The optimization results of RD process

优化参数	精馏塔
优化参数	RDC	RC
总板数	42	24
进料板	4/40	9
精馏段塔板数	4	8
提馏段塔板数	1	14
反应段塔板数	37	—
X_ProOH	—	0.80
塔径/m	1.40	0.60
再沸器热负荷/MW	2.416	0.387
冷凝器热负荷/MW	-2.022	-0.345
OC/(10⁶ CNY/a)	8.60	2.16
CC/ (10⁶ CNY/a)	7.86	1.36
TAC/ (10⁶ CNY/a)	11.22	2.08

Fig.7 Influence of feed ratio disturbance on tray temperature

Fig.8 Control diagram for composition/temperature-ratio control

Fig.9 ±10% flow disturbance dynamic response diagram

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