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

doi:10.11949/0438-1157.20230967

化工学报 ›› 2023, Vol. 74 ›› Issue (12): 4945-4955.DOI: 10.11949/0438-1157.20230967

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

李武祥¹(), 孙玉玉², 刘丹阳¹, 蔡鑫磊², 汤吉海¹^,³(), 黄益平², 张国雯¹, 张竹修¹, 乔旭¹^,³

^1.南京工业大学化工学院，材料化学工程国家重点实验室，江苏南京 211816
^2.中建安装集团有限公司，江苏南京 210023
^3.国家“江苏先进生物与化学制造协同创新中心”，江苏南京 211816

收稿日期:2023-09-15 修回日期:2024-01-02 出版日期:2023-12-25 发布日期:2024-02-19
通讯作者: 汤吉海
作者简介:李武祥（1998—），男，硕士研究生，1132291890@qq.com
基金资助:
江苏省产学研合作项目(BY20221239);江苏省重点研发计划重大科技示范项目(BE2021710);江苏高校“青蓝工程”项目

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

Wuxiang LI¹(), Yuyu SUN², Danyang LIU¹, Xinlei CAI², Jihai TANG¹^,³(), Yiping HUANG², Guowen ZHANG¹, Zhuxiu ZHANG¹, Xu QIAO¹^,³

^1.State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211816, Jiangsu, China
^2.China Construction Industrial & Energy Engineering Group Co. , Ltd. , Nanjing 210023, Jiangsu, China
^3.Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing 211816, Jiangsu, China

Received:2023-09-15 Revised:2024-01-02 Online:2023-12-25 Published:2024-02-19
Contact: Jihai TANG

摘要/Abstract

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

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

中图分类号:

TQ 225.24

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.

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.

图/表 13

图1 丙酸正丙酯反应精馏工艺流程图（1 atm=101.325 kPa）

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

表1 反应速率的指前因子和活化能

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

表1 反应速率的指前因子和活化能

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

表2 UNIQUAC模型参数

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

表3 1 atm时体系的沸点及共沸数据

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	—	—

图2 1 atm下ProOH-ProPro-H2O 的残余曲线图

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

图3 1 atm下ProPro-ProOH的T-xy相图

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

图4 序贯优化法流程框图

Fig.4 Flowchart of sequential optimization method

图5 不同循环纯度下RDC塔各参数的经济性影响

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

图6 不同循环纯度对整个系统的经济性影响

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

表4 RD工艺优化结果

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

图7 进料比扰动对塔板温度的影响

Fig.7 Influence of feed ratio disturbance on tray temperature

图8 组成/温度-比例控制的控制图

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

图9 ±10% 流量扰动动态响应图

Fig.9 ±10% flow disturbance dynamic response diagram

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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

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

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