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Study on Anionic Continuous Solution Copolymerization of Butadiene/Styrene

Author: LiHongBo
Tutor: SunJianZhong；LiuQing；WengZhiXue
School: Zhejiang University
Course: Chemical Engineering
Keywords: Solution copolymerization Styrene Anionic polymerization Mean residence time Diene Tank reactor Continuous polymerization process Active species A molecular weight distribution index Molecular weight and molecular weight distribution
CLC: TQ316.3
Type: PhD thesis
Year: 2003
Downloads: 222
Quote: 1
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Abstract


Lithium anion solution butylbenzene continuous polymerization process for the study, in the establishment of the butadiene / styrene anionic continuous solution of the polymerization on the basis of the mode test device, with n-butyl lithium (n-BuLi), tetrahydrofuran (THF ) and cyclohexane were initiator, adjusting agent and a solvent butadiene / styrene anionic continuous solution copolymerization experimental research, synthesis of styrene-butadiene random copolymer and the product was characterized. A detailed examination of the polar additive, the material to an average residence time and the polymerization temperature, etc. the copolymerization reaction conversion rate, the impact copolymer product microstructure, molecular weight and molecular weight distribution. On the basis of experimental studies, the establishment of a continuous stirred tank reactor butadiene / styrene anion solution copolymerization mathematical model and a model parameter estimation and simulation calculation. Anionic active species dynamic equilibrium behavior of the molecular weight distribution. Anionic polymerization process of continuous stirred tank reactor level fluctuations, parameter sensitivity and dynamic behavior of the reactor, in-depth research. The copolymerization experiment results show that the raise of THF / n-BuLi ratio could be significantly increased butadiene / styrene anion the continuous copolymerization reaction speed, but when of THF / n-BuLi ratio of about 70 this trend of increase slowed. With THF / n-BuLi ratio increases, the bound styrene content of the copolymer was significantly increased 1,2 structure content increase, while the decrease in the content of 1,4 structure, and when the THF / n-BuLi ratio reached about 34 after this The trend began to slow down. With the increase of average residence time of material in the monomer conversion rate increased significantly, and an increase in the molecular weight of the copolymer product. Change on the microscopic structure of the copolymer product and the molecular weight distribution of the impact is not significant, the average residence time of the copolymer product of the molecular weight distribution index is close to 2. Increasing the reaction temperature can significantly increase the speed of polymerization, the reaction kinetics constant temperature relations conforms to the Arrhenius equation. By the completely mixed Francis and a single active species assumptions, the establishment of a mathematical model of a continuous stirred tank reactor the butadiene / styrene anionic solution copolymerization. The model gives a the copolymerization reaction conversion rate and the copolymerization product of the molecular weight distribution the moments. The experimental results of model parameter estimation strike kinetic constant. On this basis, the copolymerization reaction conversion rate and the copolymer product of the molecular weight and molecular weight distribution of a simulation calculation. The simulation results are consistent with the experimental results. Zhejiang University PhD thesis simulation analysis also showed that to initiate reaction for the instant reaction, the rate of conversion of the monomers butadiene / styrene feed mole concentration _ ratio and the average residence time associated with the product of the concentration of the initiator feed. A continuous stirred tank reactor (CSTR) in the reaction mass level fluctuations on the simulation results show that the influence of an anionic polymerization process, the continuous polymerization process of the anionic material in the CSTR liquid level fluctuation will cause the outflow of material in the monomer concentration, the polymerization molecule chain length distribution with cyclical fluctuations, but compared to the monomer concentration, polymer molecular chain length distribution of the average steady-state value of the index and the difference is very small, and fluctuations relative to the average of the ratio of small anionic continuous polymerization process is not sensitive to fluctuations of the CSTR liquid level, the average residence time is longer, the smaller the impact of fluctuations in the reactor level of anionic continuous polymerization. Probability and statistical methods to establish the cumulative distribution function of the active species in the anionic active species, multi-state dynamic equilibrium system in various states, the amount of points' method of the cloth. The numerical results indicate that, and gives the function calculate the aggregate growth in different states of the active species for the product polymer molecule the greater the reactive difference, the wider the molecular weight distribution; the faster the speed of the transition between the state of the active species, the more narrow molecular weight distribution. Modeling and simulation of the reactor parameter sensitivity analysis showed that the implementation of butadiene / styrene anion continuous solution copolymerization, there is a reaction temperature of the sensitive areas of the operating parameters; theoretical analysis shows that the dynamic behavior of the reactor in a CSTR, succinic ene / styrene anion continuous solution copolymerization phenomenon of the existence of multiple solutions and periodic solutions. Under the appropriate speed trigger conditions, the solution is stable limit cycle, with the trigger speed increases, the limit cycle disappears solution stable limit cycle becomes stable focus.

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